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Guibin Jiang · Xiangdong Li Editors

A New Paradigm
for Environmental
Chemistry and
Toxicology
From Concepts to Insights
A New Paradigm for Environmental Chemistry
and Toxicology
Guibin Jiang • Xiangdong Li
Editors

A New Paradigm
for Environmental Chemistry
and Toxicology
From Concepts to Insights

123
Editors
Guibin Jiang Xiangdong Li
State Key Laboratory of Environmental Department of Civil and Environmental
Chemistry and Ecotoxicology Engineering, Faculty of Construction
Research Center for Eco-environmental and Environment
Sciences, Chinese Academy of Sciences The Hong Kong Polytechnic University
Beijing, China Hong Kong, China

ISBN 978-981-13-9446-1 ISBN 978-981-13-9447-8 (eBook)

https://doi.org/10.1007/978-981-13-9447-8
© Springer Nature Singapore Pte Ltd. 2020
This work is subject to copyright. All rights are reserved by the Publisher, whether the whole or part of the material is
concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broadcasting, reproduction
on microfilms or in any other physical way, and transmission or information storage and retrieval, electronic
adaptation, computer software, or by similar or dissimilar methodology now known or hereafter developed.
The use of general descriptive names, registered names, trademarks, service marks, etc. in this publication does not
imply, even in the absence of a specific statement, that such names are exempt from the relevant protective laws and
regulations and therefore free for general use.
The publisher, the authors and the editors are safe to assume that the advice and information in this book are believed
to be true and accurate at the date of publication. Neither the publisher nor the authors or the editors give a warranty,
expressed or implied, with respect to the material contained herein or for any errors or omissions that may have been
made. The publisher remains neutral with regard to jurisdictional claims in published maps and institutional
affiliations.

This Springer imprint is published by the registered company Springer Nature Singapore Pte Ltd.
The registered company address is: 152 Beach Road, #21-01/04 Gateway East, Singapore 189721, Singapore
Foreword

Researchers from every academic discipline strive to understand the world around them and to
solve the big problems facing humanity. When they have made new discoveries, they share
them with their peers. With respect to these objectives, environmental chemists and toxicol-
ogists are unexceptional. Sometimes, we advance the field by publishing journal articles
reporting the unexpected occurrence of a new family of contaminants, a previously unrec-
ognized response to chemical exposure or a new way of understanding toxicokinetics. At other
times, our contributions involve peer-reviewed critical reviews or perspective articles that use
existing data to propose new ways of categorizing and explaining environmental phenomena.
And sometimes progress comes in the form of a research monograph.
Unlike scientific journals, which sometimes sacrifice pedagogy for brevity and rapid
publication, a research monograph provides authors with the opportunity to fully describe the
relevant background and motivation for their work along with its importance and the future
research opportunities that their research creates. A monograph also provides its editors with a
chance to advance the field in a manner that may not be evident to the individual teams of
authors. The editors of a research monograph carefully choose the authors and topics of
individual chapters in much the same way as an artist creates a mosaic. Every individual
chapter of the monograph describes the most recent developments in a specific field, but it is
the holistic, overall view of the field that the reader gets by considering all of the chapters in
toto that advances the discipline. For the newcomer to the field, a research monograph can be a
point of entry that connects what might otherwise seem like a disconnected set of topics. For
the experienced professional, a research monograph can open up opportunities to build con-
nections and to tailor the next set of research studies to topics that can advance the overall
objectives of the community.
A New Paradigm for Environmental Chemistry and Toxicology challenges our community
to embrace a paradigm shift in the way that it operates. In the book’s final chapter, Jin, Jiang
and Li advocate for systems-level thinking to address the seemingly daunting challenge of
responsibly managing chemicals in the Anthropocene. Their call for change could not have
come from more qualified editors and it could not have come at a more opportune time. After a
period of rapid development in the 1980s, the fields of environmental chemistry and toxi-
cology have made incremental progress through the application of new analytical and bio-
analytical tools, the extension of conceptual models to new families of contaminants and the
analysis of data from long-term monitoring programs. Over the past 40 years, the number of
peer-reviewed papers in the field has increased by over an order of magnitude as more
countries join in the quest to protect the environment. But in light of civilization’s exceedance
of planetary boundaries, this is not enough.
As we learn more about the subtle impacts of chemical fate, transport and effects and as the
industry continues to produce new families of chemicals in consumer products, crop protection
products, medicines and fuels, it is becoming evident that a new approach is needed. Simply
saying that we need to transcend disciplinary boundaries is not going to achieve this goal. No
single investigator, no matter how brilliant and hardworking they may be, can master every
aspect of this complex problem. We will always need researchers who can advance an

v
vi Foreword

individual discipline by applying cutting-edge tools to advance understanding. However, if we

want to be part of the solution to the world’s problems, we have to find more effective ways to
collaborate and to apply these tools simultaneously.
This research monograph brings together some of the leading environmental researchers
interested in chemical fate, effects and treatment to create a mosaic that provides the reader
with an understanding of where the field has been and where it is going. Considered indi-
vidually, every chapter provides the reader with a thorough understanding of some of the key
issues where progress is being made in specific sub-disciplines. Considered in its entirety,
A New Paradigm for Environmental Chemistry and Toxicology lives up to its name by
providing the reader with the knowledge needed to engage in this exciting and challenging
next stage of progress in the discipline.

Grenoble, France David L. Sedlak

June 2019 Plato Malozemoff Professor
Co-Director, Berkeley Water Center
Deputy Director, NSF Engineering Research
for Reinventing the Nation’s Urban Water Infrastructure (ReNUWIt)
Director of Institute for Environmental Science and Engineering (IESE)
University of California, Berkeley, CA 94720, USA
Acknowledgements

With the tremendous developments in environmental chemistry and toxicology in the past 50
years, new theories have emerged, innovative methods have been proposed, and fresh
applications have been conducted for various environmental problems. However, we are
facing more complicated ecosystems both locally and globally. To address a series of global
environmental issues and the future health of our planet, current research has migrated from
assessments of past segregated phenomenological exposure and its effects based upon case
chemicals towards a more predictive and scientific system with generalized principles and
translational evidence that are applicable for policymakers and managers alike.
To reflect the state-of-the-art research fronts on environmental chemistry and toxicology,
we have edited a reference book to illustrate the new paradigm shift from concepts to insights.
With Springer Nature expressing interest in publishing the book, our work started in August
2018 with an initial plan of major chapter contents and potential contributors. It took several
months before we had written confirmation from most of the selected authors. As we would
like to have the book launch ceremony in August 2019 during one of the largest environmental
chemistry conferences (The 10th National Conference on Environmental Chemistry in China),
we had to set a strict deadline (31st May 2019) for the full chapter submission. Even though
several authors could not meet the deadline, we are still very pleased to have 16 chapters on
cutting-edge progress in environmental chemistry and toxicology. We are most grateful for the
authors’ dedication and contributions. It has been a great experience working with them on
these important and interesting book chapters.
There are many people we would like to acknowledge in preparing the book for publication.
Dr. Ling Jin (Research Assistant Professor of The Hong Kong Polytechnic University) pro-
vided great help in planning the book chapters and recommending leading authors. He also
helped in drafting the last chapter to summarize the recent developments in environmental
chemistry and toxicology since the publication of Silent Spring in 1962. Miss Anisha Tsang
(Research Institute for Sustainable Urban Development, The Hong Kong Polytechnic
University) provided excellent secretarial support in liaising with chapter authors, copyright
clearance, and final document submissions. Miss Cherry Ma, our Coordinating Editor at
Springer Nature China Office, offered excellent help at every stage of the book development.
We are very grateful for her patience and cooperation. We are also grateful for Mr. Leon Lee
(our summer intern from the University of East Anglia) for his careful proof read of the whole
book.
We are most thankful for Prof. David Sedlak’s remarkable and inspiring “Foreword” to the
book. We hope the readers find the collections of theoretical developments and technological
breakthroughs in environmental chemistry and toxicology useful and valuable.

July 2019 Guibin Jiang

Xiangdong Li

vii
Contents

The Exposome: Pursuing the Totality of Exposure

The Exposome: Pursuing the Totality of Exposure . . . . . . . . . . . . . . . . . . . . . . . . 3

Vrinda Kalia, Robert Barouki, and Gary W. Miller

Insights into Exposure Sources, Processes, and Impacts

In Situ Passive Sampling Techniques for Monitoring Environmental

Mixture Exposure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
Lian-Jun Bao, Rainer Lohmann, Derek Muir, and Eddy Y. Zeng
In Vivo SPME for Bioanalysis in Environmental Monitoring and Toxicology . . . . 23
Anna Roszkowska, Miao Yu, and Janusz Pawliszyn
Dose-Dependent Transcriptomic Approach for Mechanistic Screening
in Chemical Risk Assessment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33
Xiaowei Zhang, Pingping Wang, and Pu Xia
Synchrotron-Based Techniques for the Quantification, Imaging, Speciation,
and Structure Characterization of Metals in Environmental and Biological
Samples . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57
Yu-Feng Li and Chunying Chen

Modelling and Computational Approaches for Exposure, Processes, and

Impacts

High-Throughput Screening and Hazard Testing Prioritization . . . . . . . . . . . . . . 75

Caitlin Lynch, Srilatha Sakamuru, Shuaizhang Li, and Menghang Xia
Mixture Modelling and Effect-Directed Analysis for Identification of Chemicals,
Mixtures and Effects of Concern . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 87
Peta A. Neale and Beate I. Escher
Mining Population Exposure and Community Health via Wastewater-Based
Epidemiology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
Phil M. Choi, Kevin V. Thomas, Jake W. O’Brien, and Jochen F. Mueller
Mechanistically Modeling Human Exposure to Persistent Organic Pollutants . . . . 115
Frank Wania, Li Li, and Michael S. McLachlan

Solutions for Mitigating Hazardous Exposures

The Development and Challenges of Oxidative Abatement for Contaminants

of Emerging Concern . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 131
Stanisław Wacławek, Miroslav Černík, and Dionysios D. Dionysiou

ix
x Contents

Biochar for Water and Soil Remediation: Production, Characterization,

and Application . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 153
Hao Zheng, Chenchen Zhang, Bingjie Liu, Guocheng Liu, Man Zhao, Gongdi Xu,
Xianxiang Luo, Fengmin Li, and Baoshan Xing
Nanotechnology as a Key Enabler for Effective Environmental Remediation
Technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 197
Yi Jiang, Bo Peng, Zhishang Wan, Changwoo Kim, Wenlu Li, and John Fortner

Emerging Issues of Future Concern

Disinfection: A Trade-Off Between Microbial and Chemical Risks . . . . . . . . . . . . 211

Nicholas Wawryk, Di Wu, Angela Zhou, Birget Moe, and Xing-Fang Li
Plastic and Microplastic Pollution: From Ocean Smog to Planetary
Boundary Threats . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 229
Liang-Ying Liu, Lei Mai, and Eddy Y. Zeng
Size and Composition Matters: From Engineered Nanoparticles to Ambient Fine
Particles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 241
Lung-Chi Chen and Polina Maciejczyk

Transforming Environmental Chemistry and Toxicology to Meet

the Anthropocene Sustainability Challenges Beyond Silent Spring

Transforming Environmental Chemistry and Toxicology to Meet

the Anthropocene Sustainability Challenges Beyond Silent Spring . . . . . . . . . . . . . 263
Ling Jin, Guibin Jiang, and Xiangdong Li
The Exposome: Pursuing the Totality of Exposure
 The Exposome: Pursuing the Totality
of Exposure

Vrinda Kalia, Robert Barouki, and Gary W. Miller

Abstract built environment, and neighborhood-level characteristics

Environmental determinants of health need to be mea- such as access to healthy food and parks. Furthermore, it
sured and analyzed using system approaches that account includes structural policies that control access to healthcare
for interactions between different agents that can elicit a and influence other health-related behaviours and choices.
biological response. The exposome offers a useful Given how diverse the environmental health umbrella is, it is
framework to examine the totality of exposures and their not surprising that there are several definitions of what the
contribution to health and disease. Advances in exposure environment constitutes. For the purpose of this chapter, we
science, analytical chemistry, molecular biology, and define the environment as all nongenetic factors that can be
toxicology have primed us to investigate the health effects measured in the human body which may contribute to
of exposure to mixtures and concomitant exposures. variability in disease risk and burden in an individual and the
population.

1 Introduction 2 Historical Perspective

The role of the environment in disease etiology has received The effect of the environment on human health has been
increased attention over the past several years. The genome suggested for millennia. In 400 BC, Hippocrates penned “On
and genetic variations account for far less of the disease Airs, Waters, and Places” discussing the possible role of air
burden in the population than was previously thought and and water quality, and climate on human health (Hippocrates
the variation in population burden of disease is now largely 1881). The ancient Romans were aware of the adverse
attributed to nongenetic factors. A meta-analysis of 2,748 effects from exposure to lead from pipes that conducted
twin studies reported that the environmental contribution to water. Vitruvius, a Roman architect and civil engineer, noted
thousands of complex human phenotypes was nearly equal that using earthen pipes to transport water would be safer for
to that of genetics (Polderman et al. 2015). A study in health than using pipes that contained lead (Hodge 1981). In
monozygotic twins found that the average genetic risk the nineteenth century, public health efforts were focused on
attributed to 28 chronic diseases was just 19% (range: 3– preventing exposure to infectious agents in the environment.
49%) (Rappaport 2016). Using epidemiological approaches, John Snow discovered a
The environment encompasses a broad range of factors in point of water contamination as the cause of a cholera epi-
the physical world. It includes but is not limited to dietary demic in London in 1854 (Ruths 2009). These findings and
factors, exposure to infectious and synergistic organisms, others led to changes in water distribution systems, sewage
toxicant exposures through various media and routes, the treatment, and food handling in London. Water and sanita-
tion remain important environmental determinants of health
V. Kalia
G. W. Miller (&) in many developing countries.
Department of Environmental Health Sciences, Mailman School Most modern environmental epidemiology studies begin
of Public Health, Columbia University, New York, NY 10032, with observations of regional differences in disease rates.
USA
e-mail: gm2815@cumc.columbia.edu
Adverse health effects associated with exposure to air pol-
lution were discovered through atmospheric inversion phe-
R. Barouki
Unité UMR-S 1124 Inserm-Université Paris Descartes, Paris,
nomena that led to greater exposure for an extended period
France over specific geographic regions like Donora in the USA

© Springer Nature Singapore Pte Ltd. 2020 3

G. B. Jiang and X. D. Li (eds.), A New Paradigm for Environmental
Chemistry and Toxicology, https://doi.org/10.1007/978-981-13-9447-8_1
4 V. Kalia et al.

(1948), London in the UK (1952), and the Meuse Valley in for this reality, Christopher Wild formally introduced the
Belgium (1930) (Nemery et al. 2001; Bell et al. 2004; Jacobs concept of the exposome in 2005. He defined it as the
et al. 2018). Several other ecological studies were seminal in “life-course environmental exposures (including lifestyle
establishing relationships between air pollution exposure and factors), from the prenatal period onwards” (Wild 2005).
adverse health outcomes (Dockery 1753). In the 1960s–70s, The formal definition has undergone several revisions but
research focus shifted toward chemical and physical agents most versions agree that the exposome comprises the entire
in the environment that can affect human health. Several set of lifelong environmental exposures and the biological
researchers and public health agencies studied the effect of response associated with these exposures (Wild 2012; Rap-
exposure to volatile organic compounds, metals, particulate paport 2011; Miller and Jones 2014; Miller 2014). Investi-
matter, pesticides, and radiation on health. Books like Silent gating the biological response to an exposure accounts for
Spring (1962) and Our Stolen Future (1996) were critical in toxicity mechanisms and interindividual variability in
raising public awareness in the US on the societal cost of response. It also allows for the measurement of transient
exposure to persistent organic pollutants and exposures that would be invisible through traditional
endocrine-disrupting chemicals. Recently, the effects of approaches of exposure assessment. Since the environment
natural disasters, the built environment and global climate is dynamic across the life course, assessing all exposures
change on health have also been investigated. appears a daunting task. However, recent advances in
Increased research efforts in precision medicine have also methods bring optimism and avenues for creativity in the
benefited environmental health research. Advances in field.
molecular techniques have made it possible to study gene x
environment interactions that can alter disease risk. The
human genome project provided tools to make environ- 3.1 Tools to Monitor the Exogenous Exposures
mental determinants of health personalized, offering the at the Population Level
opportunity to discern how certain genotypes may be more
susceptible to effects of an environmental exposure (Collins Remote sensing is the science of gaining information on
et al. 2003). Apart from the geographical and genotypic objects from a distance and has been used to identify
context, the life stage during exposure can also alter disease exposures related to the urban environment. Specifically,
risk and susceptibility to exposure. The developmental ori- they can be used to estimate population-level exposure to air
gins of health and disease (DoHAD) hypothesis has led to pollution, changes in temperature, amount of green space
the discovery of epigenetic transfer of information from assessed using a normalized difference vegetation index, and
parent to offspring and unveiled the vulnerability of the fetus provide information on outdoor light-at-night exposure
to environmental toxicants and their effect on development (Larkin and Hystad 2018; Markevych et al. 2017; Turner
and health in later life (Barker 2007). et al. 2017; Kloog et al. 2008; Rybnikova et al. 2016).
Advances in environmental chemistry and toxicology Further, remote sensing data from a number of satellites has
have been critical in understanding environmental contrib- been integrated to determine global fine particulate matter
utors of human disease. Environmental epidemiology uses concentrations (van Donkelaar et al. 2010).
both to assign exposure and to determine the biological Mobile and stationary sensing monitors are usually used to
plausibility of observed association between exposure and make exposure measurements in specific locations. They can
outcome. be a part of national networks of measurement or be related to
study-specific measurement campaigns. National networks
tend to have limited coverage but can be used as part of a
3 The Exposome distributed sensor network, which uses low-cost sensors to fill
in spatial gaps that national networks are unable to meet.
In order to understand the mechanisms by which environ- These have been implemented in West Oakland, California
mental exposures can affect human health, researchers and (West Oakland Air Quality Study), and in Eindhoven, The
regulators have studied exposures in great detail and Netherlands (AERIAS Project). However, low-cost sensors
described the effect of exposure in isolation to a number of still require rigorous validation, limiting their widespread
chemicals on various health outcomes. However, real-world application (Curto et al. 2018). Mobile measurement cam-
exposures do not occur in isolation and are accompanied paigns have been implemented more recently in a few places,
with other exposures and context-specific factors. Besides, like Karlsruhe, Germany, and Zurich, Switzerland (Hage-
human interaction with the environment is lifelong, constant, mann et al. 2014; Hasenfratz et al. 2015).
and spatiotemporally dynamic. Most epidemiological and Modeling approaches find utility in distilling GIS and
toxicological studies do not account for this chronic, satellite data or spatial resolution. Models such as land use
low-dose exposure to environmental chemicals. To account regression, kriging, and maximum entropy models have
The Exposome: Pursuing the Totality of Exposure 5

been considered by researchers and will need to be elabo- global changes in gene expression, enzyme activity,
rated (Jerrett et al. 2010). Data generated from metabolite pathway alterations, and protein
population-level exposure assessments provides opportunity synthesis/folding. Deep molecular phenotyping can provide
to create ecological studies that can provide links between information on acute biological responses and also provide
exposure and population health. Most of these data sources, measures of long-term changes in physiology which can be
however, are ineffective at determining individual exposure viewed as markers of exposure memory (Go and Jones 2016;
levels. They will need to be integrated with individual-level Weinhold 2006; Jeanneret et al. 2014).
measures for validation. Metabolomics. The metabolome is comprised of small
molecules in a biological matrix that is <2000 Daltons in
molecular mass. It is thought of as the functional output of
3.2 Tools to Monitor the Exogenous Exposures genes and proteins, and their interaction with the environ-
at the Individual Level ment. Recent advances in mass spectrometric techniques
have made it possible to capture previously undetected small
External sensors can be used to track a myriad of personal molecules, with estimates suggesting the metabolome may
information. Personal location data obtained through GPS comprise of more than 1 million chemical features (Uppal
devices enable integration of exposure maps with individual et al. 2016). Chemical signals derived from a biological
location markers to get personal exposure estimates (Asim- sample can arise from an endogenous metabolism, envi-
ina et al. 2018). Accelerometers and other activity tracking ronmental chemical exposures, diet, the microbiome, per-
personal devices like Jawbone, FitBit, Apple Watch, and sonal care products, and drugs (Petrick et al. 2017; Liu et al.
Polar (Loh 2017) can be used to ascertain both external 2016; Jones 2016; Walker et al. 2019; Walker et al. 2016).
exposures and certain lifestyle factors related to exercise and Using an untargeted approach, metabolomics can expand
diet. Personal sensing technologies can also be used to assess surveillance of environmental chemicals, detect new xeno-
air pollution exposure, changes in ambient temperature, and biotic chemicals, and identify unknown pollutants (Bonval-
presence of green space (Nieuwenhuijsen et al. 2014). Pas- lot et al. 2013; Roca et al. 2014; Jamin et al. 2014).
sive dosimeters like silicone wristbands can also be used for Historically, metabolomics has not focused on those
personal exposure assessment and provide valuable semi- exogenous chemicals, but recent efforts are increasing the
quantitative information on several chemicals (O’Connell identity of environmental chemicals through these untar-
et al. 2014). geted approaches. By simultaneously measuring exposure
Smartphone-based sensors and assessments can integrate and biological response, metabolomics offers the opportunity
data from personal sensors like accelerometers, GPS, to link exposure to molecules associated with exposure.
barometers, thermometers, and ambient light sensors to While the identity of most chemical features that are mea-
record personal exposures. Their high penetrance worldwide sured using untargeted high-resolution metabolomics remain
provides a unique opportunity to obtain large amounts of unknown, the technique offers a powerful opportunity for
personal data from diverse individuals (Murphy and King hypothesis generation and identification of unknown chem-
2016; van Wel et al. 2017). icals of interest related to a health outcome.
Personal sensors to monitor heart rate, glucose levels, Transcriptomics. Gene expression is the process by
blood pressure, muscle activity, body temperature, and sweat which genetic data encoded by DNA is transcribed to RNA,
production are being developed and will require validation which then initiates and directs protein synthesis in a cell.
before their implementation in large population studies. Cellular function regulation involves a complex series of
Compared to measurements of external exposure, steps that control the amount of RNA, and in turn, protein
individual-level data is more actionable, can be used for that is synthesized. Thus, exposures that alter functional
personalized advice, and can be related to internal dose and regulation in the cell can be detected using transcriptomic
associated biological responses. and metabolomic analyses. Chemical exposures have been
linked with distinct gene expression profiles that have been
seen in humans and model organisms (Hamadeh et al. 2002).
3.3 Tools to Measure Endogenous Response Transcriptomic analyses in human samples involve DNA
and the Exposome microarray hybridization, which uses 40,000–50,000
molecular probes to seek RNA transcripts (McHale et al.
Techniques in molecular biology have shown exponential 2009; Spira et al. 2004; Fry et al. 2007). Next-generation
advancement in the past three decades. These advances have sequencing has made it possible to measure the effect of
increased the resolution at which biological response to exposures on different types of RNA in a sample, including
perturbations from environmental exposures is measured. mRNA, microRNA, small interfering RNA, and long
Exposures to environmental factors can induce local and non-coding RNA. Databases that curate gene expression
6 V. Kalia et al.

profiles across different exposures and model organisms cohort studies will generate data needed to spur new dis-
provide opportunities to compare experimental data with coveries and methods (Vineis 2017; Vrijheid 2014; Li et al.
previously generated gene expression profiles (Grondin et al. 2017; Barouki et al. 2018; Carvaillo et al. 2019).
2018).
Proteomics. Protein measurement can elucidate signal-
ing, inflammation, oxidative stress, and tissue damage in a 3.4 Considerations in Measuring Exposure
biological sample. Levels of proteins and their posttransla- and Biological Response
tional modifications are closer to function than gene
expression data. Measuring proteins can be targeted using We have learned several lessons from environmental epi-
enzyme-linked immunosorbent assays (ELISA), or newer demiology about associations between exposure and disease.
multiplexed bead-based assays that are capable of measuring Investigators have recognized the importance of accuracy
more than 50 proteins in a small amount of biological and precision while measuring exposure. Accurate exposure
material (Elshal and McCoy 2006; Tighe et al. 2015). While assessment is essential to detect and quantify a dose–re-
the use of high-resolution mass spectrometers in untargeted sponse relationship. Inaccuracy can lead to
proteomics is insightful, it is also challenging due to diffi- mis-measurement of a continuous exposure measure or can
culties in detecting low-abundance proteins. Chemical lead to misclassification of a dichotomous exposure status,
exposure to reactive electrophiles has been achieved through which can severely bias results toward the null. Using
protein adductomics platforms, which can measure more biomarkers of exposure has several advantages: 1. Detection
than 100 human serum albumin adducts at the Cys34 site. of the biomarker proves absorption of the compound, 2. It
Protein adductomics has been used to assess exposure to accounts for bioavailability of the compound, and 3. It
lifestyle factors, indoor air pollution, and ambient air pol- integrates measures over all routes of exposure. However, it
lution (Rappaport et al. 2012; Grigoryan et al. 2016; Liu remains hard to tell where in the environment the compound
et al. 2018). came from, positing the need to compare internal dose data
Epigenomics. Epigenetic changes on DNA can alter gene with data collected from external monitors and measure-
expression. These changes can occur through the addition or ments. Further, since biomarker collection is expensive and
removal of methyl groups on CpG dinucleotides, or through relies on access to biological matrix availability, we can also
histone modifications. These modifications can be long term validate other less expensive measurement methods by val-
and have the potential to be transferred to the next genera- idation against biomarkers measured in a subset of the
tion if they occur in germ cells. Different stressors including population. Epidemiological studies that provide causal
chemical exposures can lead to specific epigenetic signatures interpretation of observations have good study designs.
that persist even after the stressor has been removed (Fer- These study designs account for all variables that can con-
nandez et al. 2012). Thus, epigenetic profiles can be used to found relationships between exposure and response, and
monitor exposure history and to assess acute or chronic provide the means to uncover temporal relationships.
stress (Go and Jones 2016; Go and Jones 2014).
High-throughput assays based on parallel sequencing of
DNA with bisulfite conversions can measure up to 850,000 4 An International Perspective
CpG sites within the human genome. Epigenome-wide
association studies have revealed distinct methylation pat- Chris Wild’s article (Wild 2005) describing the exposome
terns associated with chemical exposures, providing insight concept raised a huge interest in the scientific community,
into the mechanisms underlying the biological responses which did not translate immediately into identified projects
(Bollati et al. 2007; Seow et al. 2014; Hou et al. 2012). in Europe until the European commission launched research
Multi-omics assessment of the exposome. Information calls on the exposome within the seventh framework (FP7).
from different layers of the biochemical dogma can be In 2012 and 2013, three projects were launched, HELIX,
integrated to paint a holistic picture of biological response to Exposomics, and then HEALS. The concept was not to
an environmental perturbation (Fig. 1). Using approaches develop facilities, but rather to form integrated projects that
from systems biology, we can gain a deeper understanding would encompass the complexity of the exposome. Each
of environmental influences on human health by integrating project had its own perspective. HELIX, for example,
across epigenomic, transcriptomic, proteomic, and metabo- focused on the pregnancy exposome by studying several EU
lomic changes associated with exposures. The integration of birth cohorts (Maitre et al. 2018), Exposomics focused on
high-dimensional data has benefited from the development the short and long-term effects of exposure to water and air
of statistical approaches that identify interactions among pollutants (Turner et al. 2018), and HEAL focused on
biological response networks (Uppal et al. 2018; Kalia et al. modeling and multidisciplinarity to develop a new “expo-
2019). The continued use of deep molecular phenotyping of some” cohort (Steckling et al. 2018). More recently, the
The Exposome: Pursuing the Totality of Exposure 7

Fig. 1 The exposome concept

Environmental exposures can
derive from individual factors
(like diet) and from general
sources (like air pollution).
Exposures that affect health leave
a biological fingerprint that can be
measured through changes in
biological response in different
biochemical layers. Integrating
measures of external exposure
and internal biological response
create the exposomic framework
to assess health status through
risk and impact assessment.
(Created with BioRender)

European Commission launched a new call within the which can help predict and identify unknown chemical
H2020 framework, which will support 4–5 projects with a signals measured in human and environmental samples.
clear focus on the development of an exposome toolbox that Efforts are underway to use high-resolution mass spec-
should be coordinated by a cluster gathering of those pro- trometers to characterize all chemicals present in an envi-
jects. It is fair to say that several other projects within the EU ronmental sample. Methods have been developed to identify
are inspired by or address one of the exposures that consti- “known unknown” chemicals using spectral fragmentation
tute the exposome (Karjalainen et al. 2017). As an example, patterns that can help deduce chemical structure and identity
the EU biomonitoring program, HBM4EU, focuses on (Schymanski et al. 2015; Gago-Ferrero et al. 2015).
chemical exposures, while the project Lifepath addresses In an epidemiological setting, Liang and colleagues used
primarily socioeconomic aspects. There are other projects high-resolution metabolomics to characterize plasma and
addressing urban exposures or the eco-exposome. While all saliva samples from participants of a traffic-related air pol-
these projects do not focus per se on technology develop- lution exposure study. They measured a number of
ments, they do allow significant technological progress, traffic-related air pollutants using external monitors and
most notably in analytical methodologies, sensor technol- measured the association between exposure and metabolic
ogy, biostatistics, and bioinformatics. Clearly, the upcoming profiles of the participants. Chemical features of interest that
exposome toolbox cluster will highlight and further develop were significantly associated with exposure belonged to
these methodologies with the aim to support public health metabolic pathways related to inflammation and oxidative
and regulatory decisions as well as informed individual stress, including leukotriene and vitamin E metabolism
prevention. (Liang et al. 2018).

5 Environmental Chemistry 6 The Exposome and Toxicology

and the Exposome
More than 85,000 chemicals are registered with the EPA for
Chemicals released into the environment usually undergo manufacture, import, and use in commercial products.
transformations under different environmental conditions to Approximately, 112,000 chemicals and compounds are
produce intermediate chemicals. Several tools have been registered with the US Food and Drug Administration as
developed (Ruttkies 2016; Djoumbou-Feunang et al. 2019) drugs or food additives (Niedzwiecki et al. 2019).
8 V. Kalia et al.

A majority of these chemicals have little information on their measure biological response (Sect. 3.3.) can be applied on a
health effects at low concentrations and their influence as cellular level to ascertain changes in gene expression, protein
complex mixtures seen in real-world scenarios. This poses a expression, metabolism, and epigenetic modifications due to
significant challenge that requires expertise across several an exposure.
disciplines. Toxicologists have been systematically working Model organisms. While cell-based assays serve as
through this list of chemicals that contribute to the chemical excellent screening tools, single cells don’t represent com-
exposome. High-throughput screening assays have gained plex tissue interactions of a whole organism. To this end,
popularity for their efficiency and the high resolution of data model organisms like Caenorhabditis elegans (worms) and
they produce. They both conserve time and provide valuable Danio rerio (zebrafish) have been gaining popularity as
insight for researchers toward the affected organ system or toxicological models. The short generation times of C. ele-
pathway that may be perturbed due to an exposure. The gans make them excellent models to study aging and life
National Toxicology Program in the US has been leading a course specific changes in response to exposure. Several
shift in current toxicological research, moving away from molecular pathways have been conserved across
in vivo testing and incorporating high-throughput in vitro evolution-making discoveries and observations in these
assays, model organisms, and computational models to study models relevant for the human context. In a metabolomic
the adverse effects of exposure to chemical mixtures study, Jones and colleagues described changes in metabo-
(Council 2007). Some of these methods are discussed below. lism in C. elegans as a result of exposure to a mixture of the
Structure–activity relationship (SAR). This method heavy metal nickel and the pesticide chlorpyrifos. The
uses physical and chemical characteristics to predict toxicity authors noted changes in metabolism of the branched-chain
based on the similar-property principle, i.e., similar struc- amino acids and tricarboxylic acid cycle intermediates. They
ture = similar biological activity (Tong et al. 2003). These also found changes in reproduction (brood size) due to
methods can be quantitative (mathematical modeling) or exposure to this mixture of toxicants (Jones et al. 2012).
qualitative (recognize substructures that afford toxic prop-
erties). They have found utility in predicting toxicokinetics,
half-lives, and the ability of chemicals to cross the blood 7 Conclusion and Future Directions
brain barrier.
In vitro testing. Human cell lines and animal cell lines Understanding the relationship between the totality of envi-
transfected to express human genes can be used to create ronmental exposures and health poses many challenges. Many
assays to measure molecular changes due to different exposures are largely involuntary and dynamic, and not all
exposures. Modifying assay parameters and changing cul- environmental exposures have been fully characterized.
ture conditions can alter the context of exposures to answer Studying the exposome thus relies on cutting-edge technolo-
specific biological questions. As an example, in vitro cell gies that can detect and identify chemicals we are exposed to,
lines have been used to study the effect of exposure to moving beyond a targeted list of known chemicals of interest.
mixtures on receptor ligand binding and activation. A group Analysis and interpretation of this data requires various data
of researchers found that at low concentrations, a combina- analytical techniques: dimension reduction techniques, data
tion of two known pregnane X receptor (PXR) ligands integration, network analysis, and longitudinal analysis to
resulted in a synergistic effect on activation of the receptor, name a few. Apart from novel data analytical applications, the
which was not observed with each chemical alone. The field will also need to think about confounders and effect
researchers suggested that the two ligands together form a modifiers when measuring associations between exposure and
“supermolecular ligand” within the ligand-binding pocket of disease. For example, how should social class or socioeco-
the nuclear receptor (Delfosse 2015). Findings such as these nomic status be treated in a model—as a confounder, effect
support the exposome concept in toxicological studies. modifier, or a determinant of exposure? Uncovering the
Cell-based in vitro assays can be used for exposome will need input from scientists working in the fields
high-throughput screens, which offer an economical way to of environmental chemistry, toxicology, exposure science,
screen a large number of chemicals in a short period. These epidemiology, molecular biology, analytic chemistry, bioin-
screens are widely accepted in the pharmaceutical industry formatics, and engineering. Thus, a multifaceted problem will
to predict therapeutic action, pharmacokinetics, interactions be best tackled with multidisciplinary research teams.
with enzymes, biotransformation, metabolic products, and
have been used to rapidly detect interactions of drugs with Acknowledgements National Institutes of Health ES023839 and
genetic polymorphisms. Further, all methods described to ES030163, Inserm, and University of Paris Descartes-USPC.
The Exposome: Pursuing the Totality of Exposure 9

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Insights into Exposure Sources,
Processes, and Impacts
 In Situ Passive Sampling Techniques
for Monitoring Environmental Mixture
Exposure

Lian-Jun Bao, Rainer Lohmann, Derek Muir, and Eddy Y. Zeng

Abstract 1 Introduction
A large number of passive sampler devices have been
developed for in situ sensing of polar and nonpolar A large number of organic chemicals are synthesized and
organic chemicals in the environment. This chapter registered, with the total number registered by government
compiles and analyzes available information on the agencies reaching almost 394,000 worldwide (http://support.
current progress in quantitation theories and technological cas.org/). Most organic chemicals can be released into the
improvements. The results show that it is critical to environment through a variety of pathways, such as direct
determine sorbent phase-water partition coefficients and atmospheric emissions and domestic, industrial, and agricul-
sampling rates of target analytes for quantitation with the tural wastewater discharge, etc., which poses potential health
equilibrium and kinetic sampling strategies. Compared to hazards to organisms and humans. Monitoring of organic
passive sampling of organic contaminants in air, overly- contaminants in the environment is necessary for examining
ing water and sediment porewater, which has been their occurrence and ecological risk though a mixture of
extensively documented, measurements of organic con- exposures. Of particular note is that gaseous or freely dis-
taminants in soil and at the air–soil interface have been solved organic contaminants are considered bioavailable for
largely unsuccessful with passive samplers. In addition, organisms. Conventional active sampling methods involve
the combination of in situ passive sampling devices and relatively complex and time-consuming procedures only
bioassays could be a promising tool for directly assessing provide instantaneous concentrations of target analytes.
air and water quality with biological effects. Comparatively, passive sampling techniques, on the principle
of “like dissolves like” with sorbent phases, are easy to
Keywords

operate and often yield time-weighted average concentra-
Passive sampling Organic contaminants Field tions. Due to a great enrichment in the sorbent phase, the
application Biological effects detection limits of a mixture of organic contaminants for
passive sampling techniques can be lower than those using
active sampling methods if the sampling costs are similar.
Because passive sampling techniques are simple to operate
and cost-effective, they have opened up a new opportunity for
in situ tracking dissolved organic chemicals including polar
and nonpolar in air, water, and sediment. For instance, the
L.-J. Bao (&)
D. Muir
E. Y. Zeng Global Atmospheric Passive Sampling (GAPS) Network ini-
Guangdong Key Laboratory of Environmental Pollution and tiated in December 2004 has conducted measurements of
Health, School of Environment, Jinan University, Guangzhou, persistent organic pollutants (POPs) and priority chemicals in
511443, China
e-mail: baolianjun@jnu.edu.cn the atmosphere with passive air samplers (Pozo et al. 2009).
The GAPS monitoring program has covered more than 55
R. Lohmann
Graduate School of Oceanography, University of Rhode Island, sites on 7 continents in urban, rural, and remote regions
Narragansett, Rhode Island, 02882-1197, USA (Koblizkova et al. 2012). In 2010, Lohmann and Muir (2010)
D. Muir called for the establishment of a monitoring network of POPs
Aquatic Contaminants Research Division, Environment and in global aquatic environments using passive sampling devi-
Climate Change Canada, 867 Lakeshore Road, Burlington, ON ces, especially with polyethylene (PE) as a sorption phase. In
L7S 1A1, Canada

© Springer Nature Singapore Pte Ltd. 2020 13

G. B. Jiang and X. D. Li (eds.), A New Paradigm for Environmental
Chemistry and Toxicology, https://doi.org/10.1007/978-981-13-9447-8_2
14 L.-J. Bao et al.

2016, two workshops, initiated by the co-authors of this

chapter and with the participation of more than a dozen
experts, were held in Guangzhou, China to discuss the key
steps for establishing the Aquatic Global Passive Sampling
network and launch the first round of global sampling activ-
ities (Lohmann et al. 2017).
Over the decades, an increasing number of in situ passive
sampler devices have been developed with different sorbent
phases. The corresponding quantitation methods have also
been established and tested in under field conditions. Some
in situ passive sampler devices, such as semipermeable
membrane device (SPMD) and PE diffusion bag, have
gradually been adopted as routine monitoring tools by local
and national government agencies (Interstate Technology
and Regulatory Council 2004; Huckins and Alvarez 2019).
To date, new materials have been synthesized and used as
novel sorbent phases (Ren et al. 2018; Zheng et al. 2018).
A recent innovation is the development of samplers using Fig. 1 Typical extraction profile of a target analyte in a passive
multi-material 3D printing to produce low-cost passive sampler’s sorbent phase (Ouyang and Pawliszyn 2008)
sampler devices with porous membranes, which were ini-
tially used for evaluating the uptake of atrazine in water
the analyte between the sorbent phase and environmental
(Kalsoom et al. 2018).
matrix. The determination of Kf is the key step for both
This chapter reviews the latest developments in typical
quantitation methods.
passive samplers for sensing polar and nonpolar organic
Over the decades, the Kf values for a large number of
chemicals in environments in an attempt to comprehend the
organic contaminants in different sorbent phases have been
current progress in quantitation theories and technological
determined and summarized in some review articles. For
improvements of in situ passive sampling devices.
example, Difilippo and Eganhouse (2010) compiled 55 ref-
erences to evaluate the experimentally determined poly-
dimethylsiloxane (PDMS)-water Kf for polycyclic aromatic
2 Quantitation Theory hydrocarbons (PAHs), polychlorinated biphenyls (PCBs),
chlorinated benzenes, DDT compounds, hexachlorocyclo-
The essential and principal objective of in situ passive
hexanes, chlorinated cyclodienes, organophosphorus insecti-
samplers is to quantify the gaseous or freely dissolved
cides, pyrethroids, carbamates, triazines, polybrominated
organic contaminants in air, water, or sediment. Generally,
diphenyl ethers (PBDEs), and BTEX at different temperatures
the quantitation methods have been developed based on the
and with different coating thicknesses of PDMS coating in
partition process of a target analyte between the sorbent
freshwater or seawater. Lohmann (2012) also summarized a
phase and environmental matrix within a passive sampler
list of Kf for PAHs, PCBs, PBDEs, organochlorine pesticide,
(Fig. 1). Here, two quantitation methods for in situ sampling
triclosan, etc. between low-density polyethylene (LDPE) and
on equilibrium partitioning and kinetically controlled diffu-
water. Recently, Lao et al. (2017) experimentally determined
sion respectively are introduced.
Kf values of 112 moderately hydrophobic organic compounds
including PAHs, PBDEs, PCBs, and pesticides between poly
(methyl methacrylate) and water. Smedes (2018) also mea-
2.1 Equilibrium Sampling
sured silicone–water Kf values of 80 organic compounds, such
as phthalates, musks, organophosphorus flame retardants,
When a target analyte in an environmental matrix (air or
chlorobenzenes, pesticides, selected PCBs, and a number of
water) equilibrates with that in the sorbent phase of a passive
miscellaneous compounds using a cosolvent method. Col-
sampler, its gaseous or freely dissolved concentration (de-
lectively, it is interesting to note that the relationships between
fined as Cf) can be derived by
log Kf and log Kow (octanol–water partition coefficients) were
Cf ¼ Cs =Kf ð1Þ established for unknown compounds in these four afore-
mentioned and other references (Bao et al. 2011; Yang et al.
where Cs is the analyte concentration in the sorbent phase at 2006). It has been debated for years whether the relationship
equilibrium and Kf is the equilibrium partition coefficient of between log Kf and log Kow should continue to be linear or
In Situ Passive Sampling Techniques for Monitoring … 15

become nonlinear as log Kow reaches 7–7.5 and beyond. directly determined from the initial and remaining amounts
Several factors, such as poor mass balance, low solubility for of the PRC in the sorbent phase and the equilibrium partition
very hydrophobic organic chemicals (VHOCs), loss of coefficient Kf. For the best calibration, the PRCs should be
VHOCs to container surfaces by sorption, nonequilibrium the isotopically labeled analogues of the target analytes. If
state, chemical molecular volume, and energy barrier for isotopically labeled PRCs are not available, unlabeled and
chemical diffusion into polymer structure have been impli- homologous chemicals which have similar physiochemical
cated as the causes for the aforementioned relationships (Lao properties with the target analytes but are seldom detected in
et al. 2017; Bao et al. 2011). Apparently, further investigations the environment can be used as PRCs. Several calibration
into the correlative relationship between log Kf and log Kow methods, such as non-linear least squares regression (Booij
are necessary and beneficial for extending the application of and Smedes 2010), molar volume adjustment (Tomaszewsky
passive samplers to nontarget VHOCs. In addition, the effects and Luthy 2008), correlation between and log Rs and log
of temperature, ionic strength, and pressure on the Kf have Kow (Yao et al. 2016), one-dimensional model (Fernandez
been reported and should also be taken into account in et al. 2009), and exposure adjustment factors (Huckins et al.
developing passive sampling methods. 2002), have been developed to estimate the Rs of a suite of
analytes without isotopically labeled PRCs. However, the
limitations of PRCs calibration methods (Liu et al. 2013a),
2.2 Kinetic Sampling such as high cost and retained fraction, have been recog-
nized. Hysteretic desorption of PRCs from PE and PDMS
Compared to equilibrium sampling, the advantage of kinetic occurred with in situ passive sampling HOCs in sediment
sampling is the relatively shorter sampling time required, porewater under stagnant conditions, resulting in anisotropic
which would somewhat reduce the likelihood for loss or exchange kinetics of PRCs and target analytes (Bao et al.
damage of passive samplers in field deployment. On the 2016; Choi et al. 2016). Such anisotropic exchange kinetics
other hand, the detection limits with the same amount of in sediment requires more complicated use of PRC-based
sorbent phase is greater for kinetic sampling than for equi- calibration methods; several of these have been detailed in
librium sampling for obvious reasons. Generally, the kinet- the literature (Fernandez et al. 2009; Sanders et al. 2018;
ically controlled diffusion process for HOCs is divided into Thompson et al. 2015). To deal with this issue pragmati-
two regimes, i.e., linear and curvilinear (Fig. 1). Within the cally, periodic agitation was introduced for in situ passive
linear uptake regime, Cf can be calculated by sampling of VHOCs in sediment porewater (Jalalizadeh and
Ghosh 2017).
Cf ¼ N=Rs t ð2Þ Besides dynamic conditions, complex environmental
where N is the analyte mass in the sorbent phase at sampling matrices also exhibit some effects on kinetic sampling. Lin
time t and Rs is the sampling rate. Within the curvilinear et al. (2018) found that the dissipation rates of HOCs from
uptake regime, Cf can be determined by PDMS fiber in water were enhanced by a factor of 70 and 34
with addition of humic acid and 2-hydroxypropl-b-cyclo-
Cst dextrin, respectively. They also developed a quantitative
Cf ¼ ð3Þ
K f (1  exp(  KRf ms t s )Þ structure–activity relationship model to associate the exper-
imental dissipation rates of the target HOCs with their
where Cst is the analyte concentration in the sorbent phase at physical–chemical properties and dissolved organic matter
sampling time t and ms is the mass of the sorbent phase. contents (Lin et al. 2018), which may be applied in esti-
Obviously, it is critical to determine Rs for estimating Cf. mating dissipation rates of HOCs in natural environments.
To in situ calibrate Rs of target analytes, the best approach Kinetic sampling is often adopted for polar organic
is to spike performance reference compounds (PRCs) into chemicals. Similar to HOCs, the quantitation methods for
the sorbent phase before deployment, assuming that the most polar passive samplers, such as ChemcatcherTM and
isotropic exchange kinetics between the uptake of the target polar organic chemical integrative sampler (POCIS), are also
analytes to the sorbent phase and the dissipation of PRCs based on the uptake profiles of target analytes in the sorbent
from the sorbent phase to ambient environment are the same. phase (Gong et al. 2018). As a result, Eq. (3) has been used
Under this assumption, Cf can be expressed as to calculate the concentrations of polar organic chemicals in
water with the aforementioned passive samplers. However, it
Cst should be noted that the PRC calibration method is not
Cf ¼ q ð4Þ
K f (1  q ) suitable for in situ calibration of the sampling rates of polar
0
organic chemicals because of the anisotropic kinetics (Gui-
where q and q0 are the amounts of a PRC at time t and 0 on bal et al. 2015; Fauvelle et al. 2012). Given the common
the sorbent phase. Equation (4) indicates that Cf can be structures of polar passive samplers, such as POCIS and
16 L.-J. Bao et al.

diffusive gradients in thin film technology (DGT), diffusive Red River from the United States–Canada border. Two
layer is usually designed to ensure that the uptake of target novel o-DGT samplers were developed, which consist of
analytes into the samplers is a linear process. Under this XAD18 and HLB, respectively, as binding phases to mea-
circumstance, Eq. (2) can be used to quantify concentrations sure perfluoroalkyl substances and organophosphorus flame
of polar organic compounds in water or sediment porewater. retardants in aquatic system (Zou et al. 2018; Guan et al.
Alternatively, the concentration of a target analyte can be 2018). Chen et al. (2015) used o-DGT samplers with a
obtained by (Davison and Zhang 1994) 0.5 mm XAD18 resin gel as a binding phase, 0.8 mm
agarose diffusive gel, and polyethersulfone filter membrane
MDg to in situ measure the concentrations and fluxes of four
Cf ¼ ð5Þ
DAt antibiotics in soils. XDA-1 resin was used as binding phase
where M is the analyte mass in the receiving or sorbent of o-DGT sampler for measuring endocrine disrupting
phase; Δg is the thickness of diffusive layer; D is the dif- chemicals in seawaters (Xie et al. 2018). Of particular note is
fusion coefficient of the analyte through the diffusive layer; that a porous carbon material from metal–organic framework
and A and t are the exposed area and sampling time, was used as novel binding gel to in situ measure antibiotics
respectively. In addition, a series of environmental factors, in water (Ren et al. 2018). The cyclodextrin polymer
such as hydrodynamic conditions, temperature, pH, ionic membrane was also adopted as the novel binding phase of
strength, and dissolved organic matter, have some impacts DGT sampler to determine the concentrations of triclosan,
on passive sampling of polar organic chemicals. These triclocarbon, and methyl triclosan in rivers (Wei et al. 2019).
issues were recently reviewed by Gong et al. (2018). Also, In summary, o-DGT samplers are an important and emerg-
standardization of the sampler layout has been recommended ing passive technique for in situ sampling of polar organic
to better calculate the sampling rates of polar organic com- chemicals and moderate HOCs in water and soil.
pounds with passive samplers (Booij and Chen 2018).
3.2 Nonpolar Organic Chemicals

3 Method Development 3.2.1 Polyurethane Foam Disk

Polyurethane foam (PUF) has been used to collect gaseous
3.1 Polar Organic Chemicals HOCs with an active high-volume air sampler. It is also
employed as a sorbent phase (PUF disk) in passive air
ChemcatcherTM and POCIS are the common passive sam- sampling—this is one of a few passive samplers that actually
plers for measuring polar organic chemicals in water. Their also collects HOCs on particles (Rauert et al. 2018; Fran-
configurations with different receiving phases or sorbent cisco et al. 2017). Generally, a PUF disk consists of two
phases have been described in previous studies (Bernard stainless steel domes or bowls with external diameters of 30
et al. 2019; Kingston et al. 2000; Ahrens et al. 2018). Here, a and 20 cm, respectively. Polyurethane foam as the sorbent
newly developed promising sampler is introduced as an phase PUF is housed inside the lower dome, and target
example of recent progress in method development. compounds in the air are allowed to freely pass through the
The emerging sampler is organic-DGT, named as o-DGT. gap between the domes and holes in the bottom surface of
In fact, DGT has been widely used to measure free elements the lower dome and sorbed into the PUF (Pozo et al. 2004).
in aquatic environments since 1994 (Davison and Zhang The domes are designed to protect the PUF from potential
1994). Recently, it was modified for polar organic chemicals damage by precipitation, particle deposition, sunlight (for
by replacing inorganic diffusive gel and receiving phase with degradation of the target chemicals), and wind. Another type
organic gels. The superiority of o-DGT over ChemcatcherTM of passive air sampler, i.e., polymer-coated glass, contains
and POCIS is the independence of sampling rates with the same shelter as the PUF disk, but has a thin layer of
hydrodynamic conditions (Challis et al. 2016). Collectively, ethylene vinyl acetate as the sorbent phase. Apparently, this
the main configurations of all o-DGT samplers are similar, PUF is supposed to sense HOCs in the gaseous phase.
with a protected filter, diffusive phase, and binding agent Abdallah and Harrad (2010) modified the PUF disk for
(receiving phase), which looks like a sandwich. The mate- monitoring brominated flame retardants in the vapor and
rials for diffusive phases and binding agents of o-DGT particulate phases in indoor air. In their design, the PUF was
samplers vary with different applications. For example, mounted from the middle of the lower dome to the top of the
Challis et al. (2018) used o-DGT sampler with a 0.75 mm upper dome and a glass fiber filter (GFF) was suspended in
Waters OASIS HLB binding gel and outer diffusive gel of the middle of the lower dome for collection of depositing
same thickness, both of which were made of 1.5% agarose, particulates. Similarly, Tao et al. (2007) used PUF and GFF
to determine 27 pharmaceuticals and 7 pesticides along the to construct a passive air sampler capable of collecting
In Situ Passive Sampling Techniques for Monitoring … 17

gaseous and particle-affiliated PAHs. The shelter is a stain- deployments while PUF-PAS deployed for 3-month periods
less steel cylinder with an upper cover and a porous bottom are able to reveal seasonal patterns quite clearly (Gouin et al.
plate, and air can easily flow over the cylinder through the 2008). XAD-2 is more dense (bulk density = 640 kg m−3
holes in the bottom plate. Particulates are trapped by the vs. 20–40 kg m−3 for PUF) and less porous (porosity = 0.41
GFF suspended in the cylinder at the height of 10 mm, while for XAD-2 vs. 0.97 for PUF) than PUFs. XAD-based pas-
gaseous PAHs are sorbed by the PUF attached to the top sives are also less likely to accumulate airborne particles
cover. The GFF and PUF are supported by backup plates than PUF-passives due to sampler design and the very small
fastened over a certain screw stem with nuts. pore diameter of XAD-2 (90Å) (Armitage et al. 2013).
Passive air samplers with PUF as the sorbent phase are Sampling rates for XAD-passives have been shown to be
the most widely used devices in field monitoring of HOCs. sensitive to temperature and thus results are often reported in
The impregnation of ground XAD resins into PUF also terms of nanograms per sampler rather than converted to
greatly improves the sensitivity of detecting HOCs in field concentrations. XAD-passives have been used for numerous
application (Koblizkova et al. 2012). The PUF disk has been studies of global air concentrations of relatively volatile
used to measure PAHs, PCBs, PBDEs, OCPs, and poly- organics such as volatile methyl siloxanes (Xu and Wania
chlorinated naphthalenes (PCNs) in the atmosphere of Eur- 2013) and perfluoroalkyl substances (Gawor et al. 2014), as
ope, Chile, and other countries (Pozo et al. 2004; Jaward well as for current use pesticides (Shunthirasingham et al.
et al. 2004a, b; Wilford et al. 2004). The sampling time of 2010).
PUF disk for chemicals with log KOA greater than 8.5 can be
several weeks or even months (e.g., 100 and 450 days) 3.2.3 Polyethylene
(Wilford et al. 2004; Shoeib and Harner 2002). Because Because of its cost-effectiveness and ease to handle, poly-
sampling rates are strongly dependent on wind speed, pro- ethylene (PE), especially low-density polyethylene (LDPE),
longed sampling time can lead to large uncertainties for has emerged as the widest applied sorbent phase for in situ
quantitative measurements (Wilford et al. 2004; Shoeib and passive samplers. Under field conditions, the structure of
Harner 2002; Tuduri et al. 2006). Additionally, small PE-based devices is often quite simple. In earlier applica-
amounts of particulates enriched with low volatile HOCs tions, bare PE films with different thicknesses ranging from
may be accumulated by the PUF disk during outdoor 25 to 100 lm (Fig. 2a) were used to sense HOCs in air,
exposure (Wilford et al. 2004; Jaward et al. 2004), under- overlying water, and sediment porewater (Cornelissen et al.
mining the measurement accuracy for gaseous HOCs. This 2008; Ruge et al. 2018; Apell and Gschwend 2016). Over
was probably the main reason for adjusting the position of the years, certain external supporting frames have gradually
PUF and adding GFF for collecting particles in modified been designed to handle LDPE films more easily or to
PUF disks (Wilford et al. 2004; Jaward et al. 2004). While determine concentration profiles of HOCs in porewater
this can undermine the measurement accuracy for gaseous and/or at the sediment–water interface. For example, Loh-
HOCs, it has major benefits for determining total airborne mann et al. (2017) designed a stainless steel cage to hold a
concentrations of semi-volatile compounds. Further studies total of 24 LDPE or silicone rubber sheets, each sized in
with dome-enclosed PUF disk samplers has demonstrated 4 cm (width)  8 cm (length), for measuring HOCs in
that they accumulate particles, ranging in size from 250 to freshwater and seawater across the globe. Oen et al. (2011)
4140 nm, with no discrimination compared to conventional fixed LDPE films to a stainless steel sediment-penetrating
PS-1-type active air samplers (Markovic et al. 2015). rod and deployed it in San Francisco Bay, California, USA
for determining vertical pore water profiles of PCBs. Lin
3.2.2 XAD et al. (2015) designed a central probe (Fig. 2c) with a tripod
XAD-2 (styrene-divinylbenzene copolymer) resins have frame for landing on sediment bed to sense concentration
long been used for high-volume active air sampling. A novel profiles of HOCs from 30 cm above to 30 below the sedi-
passive sampler using the same resin was first reported by ment–water interface. The probe is a hollow stainless steel
Wania et al. (2003). The sampler consists of a narrow tube attached with 24 depressions wrapped by PE films at
resin-filled cylinder made of a fine stainless steel mesh 2.5 cm intervals. In addition, a sampling box for collecting
placed in a protective sampling shelter with an opening at PAHs and PCBs in soil air was designed to contain LDPE
the bottom and under the cap at the top. Comparison of XAD strips strung on a carrier, which were deployed on a grate
and PUF-passives, as well as active XAD-PUF sandwich above the soil (Donald and Anderson 2017).
(high volume and low volume) sampling for pesticides in air, Our group has also developed a series of in situ passive
showed that all four yielded similar concentrations with no samplers (Fig. 2b, d, e, and f) with PE as the sorbent phase,
systematic bias among them Hayward et al. (2010). How- including open water passive sampler, multi-section passive
ever, the XAD-passive had slower update rates than sampler, sediment–water interface passive sampler, and air–
PUF-passives and thus appears to be best for long-term water passive sampler, which can be used to determine
18 L.-J. Bao et al.

isolated by stainless steel spacers of different thicknesses. In

the lower section, the sampling cells, like sandwiched LDPE
strips, are arranged vertically and isolated by stainless steel
grating panels at an identical interval of 0.2 cm. Similarly,
the air–water sampler (Fig. 2f) consists of two parts,
intending for sensing gaseous and freely dissolved HOCs in
air and water, respectively (Wu et al. 2016). For the upper
part, an external setup was designed to protect the sampler
from rainfall and photolysis of target analytes from sunlight.
Four floats are fastened in two parallel support rods to ensure
the sampler floating in water. The consecutive sampling
units are placed horizontally and separated by stainless steel
spacers of different thicknesses.

3.2.4 Silicone Rubber

Silicone rubber is a silicon–oxygen polymer with high
content of PDMS, the commonly used sorbent phase for
solid-phase microextraction. As a polymer sorbent phase,
silicone rubber has been used as different bare shapes, such
as rods, sheets, and tubes, for in situ passive sampling of
HOCs in surface water (Emelogu et al. 2013a; Silva-Barni
et al. 2019; van Pinxteren et al. 2010). It can be cut into trips
Fig. 2 Typical passive samplers based on polyethylene (PE) or
polyoxymethlyene (POM) film: a PE membrane (Adams et al. 2007);
similar to PE film and acts as the sorbent phase for the
b Passive water sampler (Bao et al. 2012); c A probe for measuring aforementioned sampling devices. It should be noted that
concentration profiles of HOCs at the sediment–water interface (Lin silicone rubber membrane is softer and sticker than PE film
et al. 2015); d multi-section passive sampler (Liu et al. 2013b); at the same thickness, thereby relatively thicker silicone
e passive sampling device for measuring sediment-water diffusion
fluxes of hydrophobic organic chemicals (Liu et al. 2013c); f air–water
rubber (often 0.5 mm) can be adopted. Compared to PE,
passive sampler for measuring concentration profiles of HOCs at the silicone rubber exhibits greater accumulation of moderate
air–water interface (Wu et al. 2016) and light HOCs and is allowed to sense HOCs with a wider
range of log Kow in water (Pintado-Herrera et al. 2016; Allan
concentrations, depth profiles, and exchange fluxes of HOCs et al. 2013).
in overlying water, sediment porewater, and sediment– Besides field measurement of organic contaminants, sil-
water/air–water interfaces, respectively. All samplers were icone rubber has been widely used in toxicological tests with
so designed to prevent large particles from adhesion onto in vitro and in vivo bioassays by exposing test organisms,
LDPE film by adding GFF and porous shield. With this genes, and cells to extracts of in situ passive samplers
protective mechanism, target chemicals are allowed to freely (Emelogu et al. 2013b; De Baat et al. 2019). For example,
penetrate through the porous shield and GFF and diffuse into Liscio et al. (2014) observed anti-androgenic effects in
LDPE phase. Specifically, the open water sampler (Fig. 2b) extracts from silicone strips, which were deployed for
is composed of a rectangular copper box with two open 14 days in a river contaminated by wastewater effluent.
frames, which are filled with two stainless steel porous Novak et al. (2018) also observed quantifiable endocrine
plates, and GFF (Bao et al. 2012). Strips of LDPE in the disruption effects in extracts of silicone rubber samplers with
copper box are fastened in a bracket of comb-like structures 5-d deployment in the Danube River. Obviously, the com-
(Bao et al. 2012). The sediment porewater sampler (Fig. 2d) bination of passive sampling techniques, not limited to sili-
consists of a series of sampling cells isolated from each other cone rubber, and bioassays may be a promising tool for
with seclusion rings (Liu et al. 2013b). The sediment pore- directly assessing water quality and identifying new and
water sampler is able to measure concentration profiles of emerging nontarget analytes with biological effects.
sediment porewater HOCs at 2 cm intervals (Liu et al.
2013b). The sediment–water interface sampler (Fig. 2e) is
comprised of one upper and one lower section, intended for
4 Conclusions
collecting HOCs in overlying water and sediment porewater,
Passive sampling techniques have been widely used to
respectively (Liu et al. 2013c). In the upper section, the
in situ measure the concentrations of organic contaminants
sampling cells are in a horizontal spiral arrangement and
in the environment, determine their exchange fluxes between
In Situ Passive Sampling Techniques for Monitoring … 19

sediment–water and air–water interfaces, and assess the Challis JK, Stroski KM, Luong KH, Hanson ML, Wong CS (2018)
biological effects with in vitro and in vivo bioassays. The Field evaluation and in situ stress testing of the organic-diffusive
gradients in thin-films passive sampler. Environ Sci Technol
determination of sorbent phase-water partition coefficients 52:12573–12582
and sampling rates of the target analytes is critical for Chen C-E, Chen W, Ying G-G, Jones KC, Zhang H (2015) In situ
quantitation with passive samplers, and the relationships measurement of solution concentrations and fluxes of sulfonamides
between log Kf and log Kow for VHOCs merit additional and trimethoprim antibiotics in soils using o-DGT. Talanta
132:902–908
research efforts. Finally, in situ passive sampling devices for Choi Y, Wu Y, Luthy RG, Kang S (2016) Non-equilibrium passive
collecting organic chemicals in soil and at the air-soil sampling of hydrophobic organic contaminants in sediment
interface need to be developed in the future. pore-water: PCB exchange kinetics. J Hazard Mater 318:579–586
Cornelissen G, Pettersen A, Broman D, Mayer P, Breedveld GD (2008)
Field testing of equilibrium passive samplers to determine freely
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 In Vivo SPME for Bioanalysis
in Environmental Monitoring and Toxicology

Anna Roszkowska, Miao Yu, and Janusz Pawliszyn

Abstract Keywords

Solid-phase microextraction (SPME) is a well-established SPME In vivo sampling Environment
sample preparation technique in the field of environmen- Toxicology Contaminants Calibration
tal and toxicological studies. The application of SPME Bioanalysis
has extended from the headspace extraction of volatile
compounds to the capturing of short-lived and unstable
components of the ecosystem extracted from the living
organism via direct immersion of SPME probes into the 1 Introduction
tissue (in vivo SPME). The development of biocompat-
ible coatings and availability of different calibration Solid-phase microextraction (SPME) was first introduced in
approaches enables in vivo sampling of exogenous and 1989 as a novel sample preparation technique for environ-
endogenous compounds from the living plants and mental analysis. Since then, SPME has received particular
animals without the need for tissue collection. In addition, attention as breakthrough “green” technology—not only in
new geometry designs such as thin-film coatings, needle the field of environmental and toxicological studies but also
trap devices, recession needles, coated tips or blades has in food analysis and biomedical research (Arthur and Paw-
increased the sensitivity and robustness of in vivo liszyn 1990; Bojko and Pawliszyn 2014; Souza-Silva et al.
sampling. Here, we present the fundamentals of in vivo 2015). One of the principal features that significantly dis-
SPME technique, including the types of extraction mode, tinguishes SPME from other techniques is that SPME inte-
geometry design of the coatings, calibration methods and grates sampling, sample clean-up, and analyte
data analysis methods used in untargeted in vivo SPME. pre-concentration into a single step, a feat which cannot be
We also discuss recent applications of in vivo SPME in achieved with the use of traditional sample preparation
environmental studies and in the analysis of pollutants in protocols. This unique integrative feature of SPME not only
plant and animal tissues in addition to in vivo human facilitates fast, simple, and efficient extraction of analytes of
saliva, breath and skin analysis. In summary, in vivo interest from a variety of matrices, its superior clean-up
SPME technique shows great potential for both targeted enables easy coupling of SPME to different instrumental
and untargeted screening of small molecules in the living methods such as GC-MS and LC-MS, among others. Fur-
organisms exposed to the surrounding environment. thermore, new advances in SPME have enabled the direct
coupling of SPME to MS for measurements of extracted
compounds, an attractive option that shortens total analysis
times while reducing errors related to sample handling
A. Roszkowska
M. Yu
J. Pawliszyn (Reyes-Garcés et al. 2018).
Department of Chemistry, University of Waterloo, Waterloo, ON, While SPME has gained considerable attraction in envi-
Canada ronmental studies as a leading method for analysis of volatile
A. Roszkowska (&) organic compounds (VOCs), the applicability of the tech-
Department of Pharmaceutical Chemistry, nique has broadened over the past few years to allow for the
Medical University of Gdansk, Gdansk, Poland
e-mail: anna.roszkowska@gumed.edu.pl analysis of a wide variety of environmental pollutants,
including pharmaceutical and personal care products
M. Yu
Department of Environmental Medicine and Public Health, Icahn (PPCPs), pesticides, and metal–organic compounds, as well
School of Medicine at Mount Sinai, New York, NY, USA as the analysis of endogenous compounds of plants and

© Springer Nature Singapore Pte Ltd. 2020 23

G. B. Jiang and X. D. Li (eds.), A New Paradigm for Environmental
Chemistry and Toxicology, https://doi.org/10.1007/978-981-13-9447-8_3
Other documents randomly have
different content
riparian right to the State of this stream has been estimated to be
worth no less than $1,000,000, just 80 per cent. of the total cost of
the entire farm. This trout-filled mountain creek will furnish the power
that will turn the wheels of industry on Rockview farm, provide the
electric light and fill other wants and still leave a surplus in reserve
power. For three miles up the beautiful valley its waters will be held
back in check until the time arrives for its use. A dam 55 feet high at
the breast will be constructed. More than six miles across the farm
and up in the mountain is a stream which will furnish 1,000,000
gallons of pure mountain water.
The question may be asked, in what relation does the warden of the
Western Penitentiary stand with his convict farm hands? He is one of
the boys. Could you but see him in the evening on the top of one of
the great hills near the merit house during the baseball game you
would be convinced of the statement. He jumps from his automobile,
flings his coat on the ground and takes a seat on the grass among
the prisoner spectators and is prepared to enjoy the game.
In the working out of this undertaking the welfare and future of the
prisoner after he has served his sentence has not been lost sight of.
This is best illustrated in the words of Warden Francies.
“Our mission is to turn out not worse men, but better men.”
 THE TREATMENT OF THE
MISDEMEANANT
[This excellent summary of the present correctional
treatment of the misdemeanant was read by Amos W
Butler, chairman of the Committee on Corrections, at the
National Conference of Charities and Corrections in
Memphis, in May, 1914.]
Who knows how many persons are confined in local jails in the
United States? Who comprehends the magnitude of the problem
involved? How many appreciate its relation to the individual, to his
family, to society?
The Bureau of the Census tells us that 452,055 persons were
committed to county and municipal prisons in 1910, under sentence
or for non-payment of fine. We call them misdemeanants. It is the
name ordinarily given one whose offense the law does not deem
sufficiently serious to warrant a State prison sentence. If the ratio of
commitments to the whole number received is the same throughout
the United States as in Indiana, it is probable that one and one-half
million people annually come under the influence of these local
prisons.
We know that jails are the spoil of partisan politics. They are
maintained largely on the fee basis. Most of them were built without
any proper idea of the purpose they were intended to serve. As a
rule they are insanitary, they lack proper provision for separating the
sexes and there is no means of employment. Often they are
crowded beyond their capacity. There is little attempt to classify the
prisoners. They congregate in the corridors and the older and more
experienced in criminal ways instruct the others in vice, immorality
and crime. In how many such institutions are women not only waited
upon but searched by men?
The late Samuel J. Barrows once remarked: “Back in 1876 a
committee of the New York Legislature said: ‘There is no one source
of crime more operative in the multiplication of thieves and burglars
than the common jail’ and that statement still remains true of a large
number of jails throughout the country.”
Many of you have heard Dr. F. H. Wines’ scathing denunciation of
these institutions. Delegates to the International Prison Congress
who visited this country in 1910 declared our local jail system as bad
as it was centuries ago in Europe. “Every jail I saw ought to be wiped
off the face of the earth,” said Thomas Holmes, secretary of the
Howard Association of London, and this was the general verdict of
these distinguished prison officials and penologists. It was the
idleness of the prisoners, the lack of fresh air, the indiscriminate
mingling, the long-delayed trials that impressed them so unfavorably.
“I asked two colored men how long they would be in and they said
they did not know; that they had waited eleven days for a trial,” said
Dr. Eugene Borel, professor of law in the University of Geneva,
Switzerland. “That is a shocking travesty of justice. In Europe a
prisoner gets a hearing within twenty-four hours.”
Yet under such conditions as these we detain hundreds of thousands
of persons:—The vagrant, the drunkard, the witness, the runaway
boy, the first offender, the hardened criminal, the man awaiting trial,
the convicted law-breaker. What can we expect but that they will
degenerate in body, mind and morals? Even where work is provided,
as is done in some larger jails and workhouses, it is under the old
contract system, which we should like to see abolished. In some
States misdemeanants are employed on the public highways.
However successful this may be in some parts of the country, it
would probably not be in conformity with the public sense in the
more thickly settled communities, or practicable to any great extent
in the more northern latitudes.
The whole question of the apprehension, treatment and release of
the misdemeanant is of tremendous importance. While prison
reforms are coming with surprising rapidity, they have been confined
largely to the felon. The misdemeanant has been neglected.
In the first place, what are the qualifications of the average
policeman? Ordinarily he is without training or experience. His
politics have usually had more to do with his appointment than any
other consideration. What part can such a policeman play in an
enlightened system of penology?
In a number of States the constitution proclaims that the penal code
shall be founded on principles of reformation and not of vindictive
justice. How far has that been interpreted in the statute laws? The
provision of most of our State constitutions that justice shall be
administered “speedily and without delay” is wholly forgotten. We
generally think that the day of imprisonment for debt is past. Yet
many jail prisoners are held for debt—the fine assessed against
them. The man of means pays his fine and goes free; the man
without money suffers imprisonment under conditions which menace
health and morals. It frequently becomes necessary for his family to
ask for help; sometimes he loses his job. If he becomes embittered,
or vindictive, need we wonder at it?
The picture is not all dark. Here and there light is breaking through.
We are coming to understand that the policeman can be a social
agent, a next friend, an instructor in obedience to the law. We are
beginning to regard as the best officer the one who makes the
fewest, not the most arrests. In some cities women are being added
to the police force, and there are police matrons, and jail matrons,
and even women judges.
“Humanizing the courts” is an expression coming more and more
into use. Instead of sending to jail men who are unable to pay their
fines, judges are releasing them conditionally and giving them a
chance to earn the money. The plan works admirably. Judges are
finding that their confidence is seldom misplaced. This principle has
been enacted into law in Massachusetts and other States.
Elsewhere it has been practiced without special authority of law. In
New York State the probation law provides for the collection of fines
on probation and also restitution on probation.
We are further coming to believe that too many persons are sent to
prison. Some States have adopted a system of probation, under
which many lawbreakers are reclaimed to society without the stigma
of a prison sentence. Probation has been successfully tried in
Massachusetts, New York and other States.
We have learned, too, the value of the farm colony for the open-air
employment of almost all classes of public wards. This has been
applied to the insane in Wisconsin, Massachusetts and Indiana; to
epileptics in New York, New Jersey and Indiana; to feeble-minded in
Massachusetts, New Jersey and Indiana; to both dependent and
delinquent children in many States, and more recently to certain
classes of prisoners, including all kinds of misdemeanants of both
sexes. What is being done at Cleveland, at Occoquan and at Guelph
is well known. The most recent development of this movement is the
New York State Farm for Women Misdemeanants. The simple,
inexpensive, yet substantial form of buildings, the freer life and the
opportunity to contribute in part at least to their own support, make it
far better for the inmates and cheaper to the taxpayer.
In Indiana the first step in this direction came about through the
establishment in 1907 of a State workhouse for women
misdemeanants as a branch of the Women’s Prison at Indianapolis.
The institution is entirely in control of women. Then the Board of
State Charities began a vigorous campaign for a state farm for male
misdemeanants. Conditions in the county jails were shown forth in
the following paragraph:

HOW PRISONERS LIVE AND LEARN IN INDIANA

COUNTY JAILS.
They live in idleness at the expense of the taxpayer.
They learn vice, immorality and crime.
They become educated in criminal ways.
They degenerate both physically and morally.
In 1913 an appropriation was secured, the land has now been
purchased, and work on the buildings will soon begin. The law
contemplates that the construction work shall be done largely by
State Prison and Reformatory men. The new institution is for men
who have a jail sentence of sixty days or more, and prisoners may
be transferred from the State institutions whenever room for them
exists at the farm. Eventually there will probably be several such
farms in the State, and this movement, with proper amendments to
existing laws, should in time do away with the use of the county jails
for the confinement of convicted offenders, and leave them only as
places of detention.
We now look forward to the time when we shall have a form of
indeterminate sentence for misdemeanants. The success of this
form of sentence for felons in Indiana as in many other States
justifies our belief that it will prove valuable in the treatment of
misdemeanants. Certainly some improvement can be made over the
present illogical short sentence, which benefits neither the individual
nor the public, in whose name he is held.
New York has already taken an important step in this direction.
Misdemeanants between the ages of sixteen and twenty-one are to
be committed under an indeterminate sentence to the reformatory for
this class of offenders, authorized by the legislature of 1912. The site
for this new institution has not yet been located. It is the purpose of
those interested to place it on a farm and to make it one of the most
complete and modern of reformatories.
Another needed reform, State control of county jails, is receiving
some attention. J. S. Gibbons, Chairman of the Prison Board of
Ireland, said: “I tell you what I think you lose sight of in this country:
That all these splendid reformatories deal with merely a drop in the
ocean compared with the county and city jails to which your
thousands of prisoners go, and where many are manufactured. We
were in exactly the same condition up to 1877 when we brought
county and city jails out from under local authorities in the United
Kingdom. We found the antecedent to all reform was State
centralization. In 1877 every prison and jail was put under central
administrative authority, and the expenses paid out of the imperial
funds. Three acts were passed simultaneously for the three
kingdoms. We then began at the bottom, closing all the superfluous
ones, and in that way we were able to close about half.”
I have the following statement from Sir Evelyn Ruggles-Brise, of
England: “The Prison Act, 1877, transferred the Local Prisons of this
Country (i.e. prisons for the confinement of all classes of prisoners
other than those sentenced to penal servitude) from the control of
local ‘Visiting Magistrates’ to that of the State. The Act came into
effect on the 1st of April, 1878, 113 Local Prisons being so
transferred. Since that date, their number has been reduced to 56. At
the time of their transfer, the Local Prison population stood at 21,030
—the highest known. From that date a continuous fall was recorded
until 1885, when the numbers reached slightly over 15,000. After a
series of fluctuations below and above this number, the population
stands at 15,000 at the present time. Relatively to the total
population of the country, the figure for 1878 represented 686
committals per 100,000, while that for the year ended 31st March
1912 was the lowest on record, viz., 439 per 100,000.”
Massachusetts, perhaps, has led the agitation in this country for
State control of county jails. In other States there has been some
publicity in favor of such action. An offender against the federal law
becomes a prisoner of the United States and is under the direction of
the federal judge. Why should one who violates a State law not be a
prisoner of the State? That is the theory that underlies the new law
for jail supervision in Indiana. Offenders against the State law have
been placed under the oversight and authority of the judge of the
circuit or criminal court, who is a State official. This judge may say
where and how the prisoner shall be detained, and if the jail is
unsatisfactory he may condemn it. He is authorized to prescribe
rules formulated by the Board of State Charities, which has
supervision of all jails and other public charitable and correctional
institutions. A violation of these rules, once entered in his order book,
is in effect a contempt of court.
While these advance steps have been taken, the reform is by no
means general. Most of the States continue to use, unchanged, the
system long since discarded in Europe, whence it came. The results
are not reformatory. On the contrary, they are destructive alike to the
individual and those with whom he later comes in contact. Local jails
are recruiting stations for our larger State correctional institutions.
We should make greater progress in reformation if we did not first
pollute the stream we are going to treat.
The outlook is not bright, but it is by no means hopeless. The evils
which exist are the natural result of the system we adopted. Let us
change the system. Let us begin at the bottom and study all the
steps in the treatment of the offender—his apprehension, detention,
trial, conviction, probation, confinement, treatment, employment,
conditional release, final discharge. Let us set as our goal:
1. A system of police recognizing character, merit, and
efficiency in the personnel and a proper social view for its
operations.
2. A prompt hearing for every person arrested.
3. The establishment of juvenile courts for all children’s
cases.
4. Provision for the care and detention of delinquent
children outside the jail.
5. A probation system for adults similar to that of juvenile
courts.
6. Separate trials for women offenders.
7. A modification of the present system of fines in order
not to discriminate against the poor.
8. Classification of prisoners, confinement of individuals
apart from each other and absolute sex separation in
county jails.
9. The prohibition of the use of the jail for any other
purpose than that of temporary detention.
10. The abolition of the fee system.
11. State control of all minor prisons.
 12. The establishment of industrial farms for the convicted
misdemeanants.
13. A form of indeterminate sentence for misdemeanants.
14. Their release on parole under supervision.
15. The abolition of contract labor.
The following members of the Committee on Corrections approve
and sign the report:

Major R. W. McClaughry
Julian W. Mack
Arthur W. Towne
Frank E. Wade
Joseph P. Byers
John J. Sonsteby
Quincy A. Myers
W. H. Moyer
A. J. G. Wells
J. A. McCullough
John H. Dewitt
Archdeacon B. M. Spurr

Mr. E. Stagg Whitin disagrees with what is said about the

employment of convict labor on public highways in the more thickly-
settled northern States.
 EYTINGE
By Charles Wheatley.
[In the State Prison of Arizona is a life prisoner who has
made a remarkable record. The Delinquent has followed
with great interest Mr. Eytinge’s business career while
inside the prison, and now, through an article from the
Ohio State Journal, presents Mr. Eytinge’s story in part.]
Down in Florence, Arizona, in the State Prison they have penned up
a Daytonian for life on a charge of murder. This man went into prison
an outcast ready to die—or rather about to be killed by tuberculosis.
He had been a “con man,” forger and all-around crook, and today,
seven years after his conviction, he occupies a prominent place in
the business world.
The man in question is Louis Victor Eytinge, born in Dayton in 1878.
At the age of three his parents separated. His mother was a talented
musician, while his father had been actor, broker and gambler.
Sometime after the separation young Eytinge went to live with an
uncle. He was educated in the First District school, Central high
school, spent two years at St. Mary’s Institute and one year at the
University of Notre Dame.
At the age of 16 Eytinge started on his life of crime by forging a
check. He went from bad to worse, and was soon known from east
to west and north to south by the list of bad paper he had left behind.
Many times his relatives kept him out of jail by straightening out
difficulties into which the young man drifted, but finally they became
tired of this and refused to have anything further to do with him.
Cut off from home’s ties, Eytinge became even more desperate and
finally ended up in the Ohio State Penitentiary following his arrest
and a daring attempt at a big jail delivery. While in the penitentiary
Eytinge was known as a “bad one” and when released it was found
that he was suffering from the advanced stages of tuberculosis. This
was at the age of twenty-seven. When relatives learned of his
physical condition they weakened in their determination to do no
more for him. They sent him to Arizona with an allowance of one
hundred dollars per month. He was to remain away from Dayton and
live within the law.
Eytinge had not been in Arizona very long, however, until he was
under suspicion of murder. A man with whom he had become quite
friendly and whom he had taken care of in a financial way was found
dead in the desert one day after Eytinge had been seen to leave the
city with him for a buggy ride. When the body was found Eytinge had
disappeared. He was found later in California and in his pockets
were some of the belongings of the dead man.
Eytinge was brought back to Arizona and placed on trial for his life.
He was convicted on circumstantial evidence after William A.
Pinkerton, one of the greatest detectives of the time, had declared
that it was improbable that Eytinge had killed the man “as his
criminal bend did not gallop in that direction.” Judge A. C. Wright, of
Phoenix, who defended Eytinge, was so sure of the prisoner’s
innocence that he went into his own pocket to pay for the appeal of
the case.
Eytinge was convicted and sentenced to life in prison. How long can
he live in prison? That was the question asked by all who had seen
him on the witness stand. Eytinge was near death’s door at the time.
His allowance had been cut off and he did not have the funds with
which to purchase fresh milk and eggs, two delicacies almost
absolutely necessary for the tubercular patient. The State prison was
then at Yuma, Arizona. It was a hell hole with its mosquitoes which
swarmed into the cells that looked out on the Colorado river. The
quarters were damp, dark and dirty, and afforded excellent means of
killing a man who at the time was ready to die.
But right there is the story. Eytinge was not ready to die. He was not
30 years old. He clung to the hope that something would bring about
his release. He wanted to live, wanted to breathe again the fresh air
of freedom and hobnob again with the pals, association with whom
had placed him behind steel bars. Eytinge was still a crook.
Enough of the crook! Let us get to Eytinge the business builder and
man. It is a great, broad jump we admit, but the telling of how
Eytinge accomplished it is a thousand times easier to do than the
battle which Eytinge himself had to go through in bringing about that
end. Seven years ago Eytinge was a crook of the first water, seven
years, mind you, and—today Eytinge is a man. He is looked up to by
professional advertising writers the country over. His business letters
are the best that are being written today. Eytinge is the star of them
all.
The strange part of this great accomplishment is the manner in
which it was brought about. Eytinge made the road light for himself.
He started out with weak hands to carry the torch that showed him
the way. Today Eytinge is his own light; he has thrown away the
torch and walks alone. Honesty is his greatest asset, and it was
through the writing of business letters that Eytinge found his way.
When Eytinge entered the State prison he realized that he must find
some means of making money. One could not forge checks in
prison. Eytinge was placed in the chronic ward. Around him were
Indians, Mexicans and others who in their spare moments made hat
bands, watch fobs and other articles out of horse hair. They
decorated these with rosettes hammered out of Mexican dollars.
These articles were sold whenever possible to chance visitors at the
prison, but it was a slow way of making money.
And then one day the big idea came to Eytinge! Opportunity knocked
on the steel bars and Eytinge was there to talk to Her! The crude
handiwork of the prisoners was the vehicle by which Eytinge began
to make his way. He began by writing letters to retail dealers on the
outside asking them to take the agency for the hat bands, belts,
watch fobs and other articles. It was not long until the money began
to pour in. There was a big demand for the articles, but it was the
letters that Eytinge had written that opened up the field. In these
letters Eytinge had given the dealers a straightforward account of
what the articles really were. He told the truth absolutely and
unvarnished, and one day he discovered that he had been doing
this.
Does honesty pay? This was the question that Eytinge asked
himself. He did not have to ask others—he had the proof before him.
He had discovered that honesty did pay and that it paid well. But just
at that time this new business received a severe setback. Prison
officials became suspicious that many of the letters going out from
the prison were not what they purported to be. Some of the
salesmen were suspected of filling their letters with fake statements
which were little short of appeals for help.
Word went out from the warden’s office that each prisoner could
write but two letters a week. Eytinge had been dealing with forty
retail merchants. Many a man would have thrown up the sponge and
quit. To have thirty-eight customers taken away in that manner would
have proved a shock that few concerns would have been able to
withstand. But Eytinge did not admit defeat. He soon recovered from
the shock and saw that something must be done. Two letters must
be made to do what forty had been doing before.
The wholesale field was the only thing left. Eytinge began again
through that channel. And the letters he wrote! They were full of
business from the “Dear Sirs” to the “Yours Very Truly.” These letters
did not whine. Eytinge did not have the time nor space for that. He
had to talk business, and he talked it so well that it was not long until
the two letters were doing all that the forty had ever done.
In the meantime a new administration had taken hold of affairs in
Arizona. The State prison was removed from the banks of the
Colorado up the Gila Valley to Florence, and with this change came
a change for the better in Eytinge’s health. When he entered the
penitentiary at Yuma he weighed 119 pounds and now he weighs
190 pounds, is the picture of health and physicians declare that he is
cured of tuberculosis.
Finding himself had given Eytinge two things. It gave him a new self,
one of which he was as ignorant of as you or I, and it also gave him
health. The necessity for money with which to fight off death had
done this and it had been his desire for money that had placed him
in a position where he had to get it by some other means than by
placing some one else’s name on a check.
By this time Eytinge’s letters had begun to attract the attention of
people other than those with whom he was dealing. He had become
a student of criminology also, and when Governor George P. Hunt,
the first Statehood governor of Arizona, began his fight for better
penal laws after his inauguration in February, 1912, Eytinge had
published a booklet of which he was the author, dealing with this
question. A noted sociologist has pronounced this to be the cleverest
thing ever published on the question.
Magazines soon began to find Eytinge a man worth telling their
readers about. Advertising booklets such as “Letters,” published in
Chicago; “Printers Ink,” and others sent men to Arizona to “write
Eytinge up.” In this way he became well known to men who held high
positions in the advertising field. His advice was sought by business
houses whose sales forces needed bolstering up, and he has also
been offered numerous positions as business manager and business
counsel.
Eytinge has made thousands of dollars out of his business since in
prison, but in an article a fellow prisoner has written about him it is
said that Eytinge is in debt. Why? Well, principally because he is a
man, and goes out of his way to help others. These laws of ours give
a discharged prisoner a five-dollar bill and a cast-off suit of clothing
when he starts out to face the world. Eytinge says this is not enough,
and thousands agree with him, so when he sees a man leaving
prison who is deserving and in need, he is the first to come forward
with financial aid. He has helped hundreds of men fight through the
courts for their freedom, and the families of hundreds of prisoners
can thank Eytinge for money that has tided them over the prison
term of the head of their house.
Don’t forget that Eytinge now before you is the man who seven years
ago entered the penitentiary many thought to die. Yes, the old
Eytinge is dead—Eytinge, the crook, has passed away, but it has left
an Eytinge whom the world will be glad to greet. Peter Clark
Macfarlane, a Collier’s writer, says this of Eytinge: “They had penned
him up to die. They sent him to jail, a crook, and lo, his voice was a
power for honesty.”
That is the way Eytinge is spoken of by hundreds who have become
acquainted with him through correspondence and the few who have
taken the trouble to visit him in his work shop. Among Eytinge’s first
really influential friends after he got on the right track were McCrary,
the old parole clerk at the prison, and J. J. Sanders, the new parole
clerk, who was appointed when Governor Hunt made Robert B. Sims
warden of the institution. Sims had never had any dealings with
prisoners or penitentiaries before, but he had some ideas as to how
they should be run. One thing that he remembered, which the
wardens of many States seem to have forgotten, is that prisoners
are human beings.
These three men helped Eytinge to pull himself up out of the rut. He
was made a “trusty” and given a clerkship in the parole clerk’s office.
These were about the first honest men Eytinge had ever associated
with. Honest men to him up until that time were “rubes” and “dubs”
whose money he looked upon as his own. But in his efforts to help
the parole clerks guide the footsteps of the prisoners who had been
given a chance through the parole law, Eytinge found that happiness
can come to a man by doing something for someone besides
himself.
Lecturing did not bring these things about. It was the man’s ability to
see for himself, and his horizon was the prison walls. Here he saw
before him hundreds of men who had violated the laws of society,
and he saw also that the happy ones were those who had violated
no laws but were trying to help those who had. Step by step Eytinge
was bringing himself up out of the mud. He declares today that the
happiest moments of his life were those in which he found that he
was regaining the confidence of those who had lost all faith in him.
One of the best indications of the regard in which advertising men of
the country hold this prisoner is the fact that a paper written by him
was read during the convention of the Associated Advertising Clubs
of America, which was held at Toronto, Canada, June 21-25. This
paper received greater applause than any other read before the
convention, and the delegates were so enthusiastic over it that they
voted to send Eytinge a vote of thanks.
The paper was read on Thursday at the close of the sessions when
many of the visitors were anxious to get away for their homes, but
300 men remained in the hall in rapt attention while the paper was
being read. A storm of applause swept through the hall as the reader
concluded the message from the man who “puts his brains in an
envelope.”
It has been a long, hard struggle for Eytinge. Will it win him his
freedom? That is the question many are asking. No one can tell.
Perhaps the law will unbend and open the gates to him sometime.
Those who know him are hoping that such will be the case, and
many are already doing what they can to bring about this result. That
Eytinge has hopes that such a thing will come about goes without
saying. He has served the average length of time that a “lifter”
serves in Ohio, and he is a better man than many of those who are
now released from prisons through pardons or influence.
 EVENTS IN BRIEF
[Under this heading will appear each month numerous
paragraphs of general interest, relating to the prison field
and the treatment of the delinquent.]
The Ethics of Governor Blease.—The executive of South Carolina,
who has pardoned 1200 convicts in three years, has written about it
all. Here are some of the reasons he gives for pardons.
In telling why he paroled a negro named Sam Gaskins, convicted of
manslaughter, the Governor wrote:
“This negro, being engaged to a negro girl, called to see her and in
fooling with a pistol it went off and killed her. It seems to have been a
very sad accident. However, after a second thought, possibly it was
for the good of humanity, for had they married no doubt they would
have brought forth more negroes to the future detriment of the
State.”
In explaining why he pardoned J. Allen Emerson, a white man, who
was serving a life sentence for murder, he said that the imprisonment
of Emerson had seriously impaired the health of the man’s sister.
“Her life,” the Governor states, “is worth more to her and her children
and is worth more to the citizenship and motherhood of this country
than the incarceration of her brother is worth to the State.”
In pardoning Roland Parris, who was convicted of assault and
battery on his brother-in-law, with intent to kill, the Governor explains
that Parris was protecting his sister from abuse. “I congratulate him,”
the Governor says, “for being man enough to protect his sister from
a drunken husband; in fact, I think there should be an appropriation
made by which the Governor could award him a gold medal of honor
for his action.”
The Governor thinks that if any white man calls another a certain vile
epithet and is killed the verdict should not be greater than
manslaughter. If a negro applies the epithet to a white man he
doesn’t care to say what he thinks the verdict ought to be, but
“people may draw their own conclusions.”

Germans to See Prisons.—An unofficial tour of inspection of

American prisons and reformatories by Prussian Government
officers will be made during the month of August. The Prison
Association of New York has been asked to arrange the details of
the proposed tour. The chairman of the delegation will be Dr. Karl
Finkelnburg, who for many years has been prominent as a German
prison warden, and who has recently been promoted to the position
of director of Prussian prisons under the Ministry of the Interior, a
position which had been occupied by the late Dr. Krohne.
Dr. Finkelnburg, who will arrive upon the Imperator about the end of
the first week in August, will be accompanied by Professor
Darmstaedter, of the University of Berlin, and also by a member of
the Prussian Parliament. The tour of correctional institutions will
cover a period of thirty-five days, during which time many of the most
important prisons and reformatories of the Eastern and central
positions of the country will be visited.
In recent years American correctional institutions have been
frequently the object of careful study by foreign countries. In 1910,
several hundred foreign delegates not only attended the International
Prison Congress at Washington, but made a ten day’s tour, by
invitation of the Federal Government, of many institutions. In 1913 a
tour of inspection was arranged for four official representatives of the
Prussian Government—Messrs. Plaschke, Schlosser, Hiekmann,
and Remmpis. During a month and a half nearly fifty separate
institutions were carefully inspected. The official report to the
Prussian Government of these gentlemen has not yet been received
from that Government by the United States.
The German Government is discussing the proposed revision of the
penal law of Germany. Some of the most modern and successful
features of American prison and reformatory management are being
carefully considered in this connection.

A “Relic of the Dark Ages”—So the American newspaper

correspondents called the Vera Cruz prison in Mexico.
Most famous of all Mexico’s prisons, noted for the untold
thousands tortured within its walls, the castle prison of
San Juan de Ulua, stands today on a little island
overlooking Vera Cruz pretty much as it stood in the
centuries of its existence. On April 28 the flag of Mexico
fluttered down from its flagstaff. The stars and stripes rose
in its place as Captain Paul Chamberlain and a company
of marines from the North Dakota took possession.
In his despatch to the navy department reporting the
taking over of the fortress Rear Admiral Fletcher said:
“The prison has been taken over under mutual agreement
made between myself and Colonel Vigil, in charge, which
agreement was signed and approved by Admiral Badger.
There are in the prison 43 prisoners who have been
sentenced for crime, 75 who have been accused of crime
but have not been brought to trial and also 325 who have
not been accused of any misdemeanor whatever. These
325 were arrested mostly within the last two months in
order to be forced into the federal army and for no other
reason. The above data were obtained from the officer in
charge. The conditions in the prison under which the 325
men are living are described as frightful.”
Secretary Daniels directed the release of these 325 men,
ordering that the seventy-five awaiting trial should be held
pending investigation by the American authorities into the
charges against them.
 “No stage manager putting on ‘The Count of Monte Cristo’
could imagine anything more creepy than the sight which
met the eyes of the American officers when the keys were
turned in the rusty locks and they entered the ancient
vaults,” wrote an American newspaper man describing his
visit to the prison.
In the grim, forbidding, gloomy pile of San Juan de Ulua
the Spanish inquisitors found a building suited to the
purposes and one which appealed to their torture-loving
tastes. Only a fifteenth century Spaniard could have
designed such a castle.

First Field Day at Auburn (N. Y.) Prison.—Despite several hundred

light cases of Scarlet fever, at the century old prison at Auburn “on
Memorial Day traditions were set aside when the 1,400 prisoners
there were given three hours in which to loaf or play and enjoy
themselves in the open air,” says the Poughkeepsie Press. “At two
o’clock in the afternoon they were marched into the yard in their
usual companies, and at a bugle signal they were disbanded. Then
they played baseball, and participated in other outdoor sports. There
were cheers for the winning contestants and a good time generally.
At the end of the three hours the bugle sounded the recall, the
companies were formed again, and when the men marched back
into the prison there was not a prisoner missing, and there had not
been a single infraction of discipline.
“In this instance the short outing was a complete success. It did not
destroy discipline, nor will it tend to create the supposition that the
men are pampered at Auburn.”

Road Making in New York.—In accordance with the policy of the

State Prison Department and by means of an appropriation made at
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