Sensors and Actuators B 142 (2009) 28–32

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Sensors and Actuators B: Chemical

journal homepage: www.elsevier.com/locate/snb

Flexible humidity sensor in a sandwich configuration with a hydrophilic

porous membrane夽
Yoko Miyoshi a , Kumiko Miyajima b , Hirokazu Saito c , Hiroyuki Kudo b , Toshifumi Takeuchi d ,
Isao Karube e , Kohji Mitsubayashi b,∗
a
Faculty of Information Sciences, Hiroshima City University, Japan
b
Department of Biomedical Devices and Instrumentation, Institute of Biomaterials and Bioengineering, Tokyo Medical and Dental University, 2-3-10 Kanda-Surugadai, Chiyoda-ku,
Tokyo 101-0062, Japan
c
Department of Mechanical Engineering, Tokyo National College of Technology, Japan
d
Graduate School of Science and Technology, Kobe University, Rokkodai-cho, Nada-ku, Kobe 657-8501, Japan
e
Katayanagi Advanced Research Laboratories, Tokyo University of Technology, 1404-1 Katakura, Hachioji, Tokyo 192-0982, Japan

a r t i c l e i n f o a b s t r a c t

Article history: We constructed a wearable and flexible humidity sensor (thickness: 80 ␮m) in a sandwich configuration,
Received 14 August 2008 with a hydrophilic poly-tetrafluoroethylene membrane placed between two gold deposited layers, using
Received in revised form 22 May 2009 soft-MEMS techniques. The device was used to measure humidity level, via its electrical conductivity,
Accepted 12 July 2009
using a multi-frequency LCR-meter at frequencies ranging from 100 Hz to 100 kHz. The device was cali-
Available online 21 July 2009
brated at 100 Hz against moist air over the range of 30–85% RH, which includes normal humidity levels
in the atmosphere and physiological air such as breath and evaporating sweat. The response sensitiv-
Keywords:
ity of the humidity device was extremely high, even for recovery to dry air; for example response time
Humidity sensor
Porous membrane
was less than 1 s for a conductivity shift between humid air of 80% RH and dry air of −60 ◦ C dew point.
Flexible The sensor performance was reproducible over multiple measurements, with a coefficient of variation of
Wearable 1.77% (n = 5). The sensor was appropriate for physiological applications, and was successfully used in two
Physiological humidity non-invasive approaches: to monitor breath air at the mouth, and to measure sweat moisture from the
nostrils.
© 2009 Elsevier B.V. All rights reserved.

1. Introduction applications, e.g. measuring sweat at the skin surface for mental and
physical analysis [10,11] or expired air from nostrils for the assess-
The detection and quantification of gaseous substances, such ment of sleep apnea syndrome (SAS) [12,13], flexibility (softness
as moisture, odors, and toxic and combustible gases with high and wearability) and quick response times are important consid-
sensitivity and selectivity are required in many fields. Various erations in the design of novel humidity sensors to be used in the
kinds of humidity (moisture) sensors (conductimetric, capacitive, non-invasive assessment of physiological moisture.
impedance spectroscopic, piezo-resistive type, etc.) were devel- In this study, we constructed a flexible and wearable humidity
oped as solid transducers [1–5]. Conventional humidity sensors sensor using a porous membrane with soft-MEMS techniques. The
with an interdigital capacitance (IDC) structure for a skin mois- performance of the device (calibration range, response capability
ture analysis have been fabricated by using printed circuit board and reproducibility) was evaluated using a batch flow measure-
(PCB) technology (which simplifies the bonding technique and ment system. We also used the wearable sensor in two non-invasive
reduces the cost) on the hard substrate [6,7]. An optical humid- physiological applications: to monitor the breath air at the mouth,
ity sensors have been also constructed by coating hydrogels and the sweat moisture from nostrils.
(poly-hydroxyethyl methacrylate, poly-acrylamide, poly-N-vinyl
pyrrolidinone) and nanostructured sensitive polymers onto the side
2. Experimental
surface of the optical fiber [8,9]. From the viewpoint of physiological
The structure and the photograph of the wearable humidity sen-
sor are shown in Fig. 1. At the first step, gold electrodes were formed
夽 Paper presented at the International Meeting of Chemical Sensors 2008 (IMCS-
directly by use of vapor deposition onto both sides of a hydrophilic
12), July 13–16, 2008, Columbus, OH, USA.
poly-tetrafluoroethylene (H-PTFE) membrane (JGWP14225, thick-
∗ Corresponding author. Tel.: +81 3 5280 8091; fax: +81 3 5280 8094. ness: 80 ␮m, pore size: 0.2 ␮m; Nihon Millipore Ltd., Tokyo, Japan)
E-mail address: m.bdi@tmd.ac.jp (K. Mitsubayashi). without chemical treatment and/or pre-deposition using harmful

0925-4005/$ – see front matter © 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.snb.2009.07.014
 Y. Miyoshi et al. / Sensors and Actuators B 142 (2009) 28–32 29

Fig. 1. Structure and photograph of a wearable humidity sensor shaped by knife into a 3-mm wide.

substances such as nitric acid and chromium. This H-PTFE mem- thus, application to one side was sufficient to coat and electrically
brane offers chemical stability, tear resistance, and flexibility. The insulate both gold electrode layers, allowing the dipped membrane
thickness of each gold electrode layer was 2000 Å. Deposition thick- area to function as an electrical lead. Cyanoacrylate adhesive infil-
ness was monitored continuously using a piezo-electric crystal tration was also used to separate the narrow strip membrane into
placed next to the target. Electrodes on both sides were spaced at three areas: sensitive area (length = 5 mm), lead area and electrical
equal intervals across the soft H-PTFE membrane. The gold coated terminal area of the wearable humidity sensor.
membranes retained their flexibility after vacuum deposition. After inspection of electrical shorts and washing using 80%
As the next step, the gold coated membrane was shaped by ethanol solution, the flexible sensor was stored at room temper-
knife into a 3-mm wide strip. In order to isolate a sensitive area ature except when in use for measurement.
(length = 5 mm), a cyanoacrylate adhesive developed for medical The behavior of the sensor was calibrated using a batch flow
use (Aron Alpha A “Sankyo”, Sankyo Co. Ltd., Tokyo, Japan) was measurement system (Fig. 2). Standard moist air was supplied from
applied to the middle part of the narrow strip membrane and a hand-made humidity generator constructed using an ultrasonic
dried at room temperature for 1 h. Because the H-PTFE membrane humidifier with a piezoelectric ceramic. A mass flow controller sys-
is hydrophilic and the deposited gold layers are porous, the liq- tem was used to adjust the flow rates of standard dry air and the
uid cyanoacrylate adhesive could infiltrate through the membrane; humid air supplied from the moisture generator, thus permitting

Fig. 2. Experimental set-up for the humidity measurement by using the wearable humidity sensor and the commercial available sensor.
30 Y. Miyoshi et al. / Sensors and Actuators B 142 (2009) 28–32

Fig. 3. Schematic diagram of human-breath monitoring using the wearable humid-

ity sensor.
Fig. 4. Calibration curve (semi-logarithmic plot) of the wearable humidity sensor
in moisture gases varying humidity. X-axis (electrical conductivity of the humidity
sensor) is expressed as a logarithmic scale.
the humidity levels into the sensor cell to be varied. The final flow
rate of the apparatus was 200 ml/min.
The humidity was assessed by the electrical conductivity of the deduced by regression analysis according to the following equation:
wearable device. The sensor conductivity can be measured using
either alternating current or direct current methods [14,15]. A four-
probe method using alternating current was used to avoid problems conductivity (S) = 7.50−25 [relative humidity(% RH)]10.31
resulting from electrode polarization. The humidity sensor was
At room humidity and physiological moisture concentration (i.e.
connected to the measurement system using a grip-type connec-
sweating, expiratory air, etc.), the measurement has adequate sen-
tor [14]. A computer-controlled multi-frequency LCR-meter system,
sitivity. When the sensitive area of the device was varied between
using the four-probe method at frequencies between 100 Hz and
15 and 900 mm2 , the output conductivity was proportional to the
100 kHz, was used to measure the output signals [impedance ()
sensitive area’s dimensions, but there was no effect on the slopes
and phase angle (◦ )] at the wearable humidity sensor, and to calcu-
of the calibration plots; this is consistent with previously reported
late the electrical conductivity (S) which represents the reciprocal
results [14]. The humidity sensor was constructed in a very simple
of the electrical resistance (). A commercially available humidity
manner, by first depositing Au on both sides of the porous H-PTFE
sensor (TRH, Shinyei Kaisha, Kobe, Japan) was also used simultane-
membrane and next coating with medical adhesive, thus obtain-
ously in the measurement system in order to verify the humidity
ing good softness, flexibility and safety for applications involving
of the applied air; the measurements made using the two devices
contact with the skin surface.
were compared.
Fig. 5 shows the typical response of the wearable sensor to a
Physiological applications of the wearable humidity sensor
repetitive humidity test. Moist air (80% RH) and dry air [less than
included breath monitoring and sweat detection. Fig. 3 contains
−60 ◦ C dew point (10.66 ppm)] were alternately applied at 3-s inter-
a schematic diagram of human-breath monitoring using the soft
vals to the humidity sensor using the gas flow measurement system.
humidity sensor. The wearable sensor was used to measure expired
As the figure indicates, the response sensitivity of the flexible device
air from healthy male volunteers with no history of respiratory
was much higher than that of the commercial available humidity
diseases. The humidity sensor was attached to the mouth of the vol-
sensor, in particular for recovery time in dry air [16,17]. The reason
unteer by adhering the sensor lead (non-sensitive area) with tape.
for the high degree of responsiveness may be the thin and porous
After obtaining their prior consent volunteers were instructed in
structure of the device. Because the H-PTFE membrane functioned
advance about how the determination was to be performed, and
were then asked to behave naturally while lying in a prone posi-
tion. The measurement of sweat secretion was also achieved by
attaching the wearable device onto the first fingertip.

3. Results and discussion

The sensor with the thinner structure (thickness: 80 ␮m) pos-

sessed softness, flexibility, tear resistance, and chemical stability
(Fig. 1, photograph). The calibration curve (semi-log plot) of the
wearable humidity sensor, sampling at 100 Hz frequency in moist
air of varying humidities with temperature maintained at 25 ◦ C, is
shown in Fig. 4. In order to inhibit the effect of the permittivity of
moist water with increasing the reactance of the device at highly
frequency (over 1000 Hz), the frequency applied to the wearable
sensor was chosen to be 100 Hz for the humidity measurement.
As the figure indicates, the electrical conductivity (S: siemens) was
Fig. 5. Typical responses for humidity measurement using the wearable humidity
related to the relative humidity (% RH) on a semi-log plot over a sensor applied periodical moisture air (approximately 80% RH) for every 3 s with 6 s
range of 30–85% RH (Fig. 4), with a correlation coefficient of 0.998 interval.
 Y. Miyoshi et al. / Sensors and Actuators B 142 (2009) 28–32 31

ure contains a schematic diagram of subject’s first finger, to which

the sensor tip of the wearable device (thickness: 80 ␮m, width:
1.8 mm) was attached directly. As the figure indicates, the conduc-
tivity of the humidity sensor increased rapidly after the subject
intentionally held their breath for 30 min thus, the sensor was capa-
ble of detecting sweat secretion from the fingertip gland induced
by physiological stress. The wearable humidity sensor was success-
fully used for the breath monitoring and the sweat detection as the
non-invasive physiological applications.

4. Conclusions

The wearable humidity sensor was constructed using gold

deposited onto H-PTFE membrane without chemical treatment
and/or pre-deposition using harmful substances such as nitric acid
and chromium. Thus, the device has the dual advantages of struc-
Fig. 6. Typical responses of breath monitoring for the humidity measurement in tural simplification and non-toxicity. Deposited gold adhered to the
expired air using the wearable humidity sensor for healthy male subject in lateral
membrane and could not be peeled off by mechanical stress such
position.
as bending. The gold deposited membranes retain their flexibility
even after vacuum evaporation. It follows from these results that the
as intermediate of the sensor is hydrophilic, thin and porous (thick- optimum range of humidity level for moisture measurement using
ness: 80 ␮m, pore size: 0.2 ␮m), and the gold deposited layers on the wearable humidity sensor at 100 Hz AC frequency is from 30 to
both sides of the sensor are porous and thin (2000 Å) [14], moist 85% RH (includes the physiological humid range of interest) with a
air could infiltrate through the sensor membrane and brush past high response sensitivity. The wearable sensor was demonstrated in
the porous device, resulting in the high response sensitivity. As two types of non-invasive physiological applications: breath mon-
the figure indicates, the sensor performance was reproducible over itoring and sweat detection.
multiple measurements, showing the highly reproducibility with
a coefficient of variation of 1.77% (n = 5) which is consistent with
previously reported values [less than 4% (n = 5)] in test solutions. Acknowledgements
As one of the physiological applications, the wearable humid-
ity sensor was applied to breath monitoring. Using the sensor, we This study was supported in part by TATEISHI Science and tech-
were able to measure expired air from healthy male volunteers in nology Foundation for Research Grants, by JSPS (Japan Society for
the prone position. Fig. 6 shows the typical responses of breath the Promotion of Science) Grants-in-Aid for Scientific Research Sys-
monitoring for the humidity measurement in expired air using tem, by JST (Japan Society and Technology Agency) and by MEXT
the wearable humidity sensor. As the figure indicates, because of (Ministry of Education, Culture, Sports, Science and Technology).
its rapid responsiveness, the humidity sensor is suitable for obse- Special Funds for Education and Research “Advanced Research Pro-
quiously monitoring the moisture change in expired air. The average gram in Sensing Biology”.
respiratory rate was ∼9 times/min which was calculated from 45
sensor peaks over the course of a 5-min experiment. References
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Isao Karube is a president of Tokyo University of Technology. He is also an emeritus

Biographies professor of University of Tokyo. He is a specialist of biosensor, chemical analysis,
biotechnology, bionics, etc.
Yoko Miyoshi had been a researcher graduate student at Hiroshima City University.
She had investigated the development of humidity sensors. Kohji Mitsubayashi is a professor of Tokyo Medical and Dental University (Depart-
ment of Biomedical Devices and Instrumentation). He received his Ph.D. in 1994
Kumiko Miyajima is an engineering official of Tokyo Medical and Dental University from University of Tokyo. His research interests include wearable chemical sen-
(Department of Biomedical Devices and Instrumentation). Her research interests sors for human monitoring, a newly olfactometric system using biological materials,
include immunoassay and clinical engineering. biomolecular and medical devices, microsystem technology, etc.