peer-reviewed filLers

Developing a new paradigm

for linerboard fillers
YULIN ZHAO, DONGHO KIM, DAVID WHITE, YULIN DENG, TIMOTHY PATTERSON,
PHIL JONES, EDDY TURNER, and ARTHUR J. RAGAUSKAS*

ABSTRACT: The goal of this research is to develop practical, cost-effective bonding clay fillers that improve
existing sheet properties while decreasing overall materials cost. This work represents a paradigm change in filler
use in linerboard and other grades. The innovative starch-coated filler technology allows at least 5%-10% filler con-
tent for lightweight and board grades, providing needed optical properties without detrimentally affecting physical
strength of papers. This offers a low-cost approach to significantly increasing sheet filler levels, leading to higher
strength and potentially improved printability. Results, including pilot trials, demonstrated significant improvement
in the bonding and bulking capabilities of modified clays coated with starch. The pilot data also indicated potential
for increased dewatering as filler content is increased, which can lead to higher production for dyer limited liner-
board mills.
Application: This research will help paper and board manufacturers to increase filler content and improve sheet
qualities, while reducing material costs.

S ubstituting fibers with mineral fillers in paper stock

has been practiced since the eighth century [1].
This technology has matured rapidly over the past three
bond polymer to fillers. The surface of fillers has been modi-
fied to improve filler-fiber bonding using epichlorohydrine
and polyamino-amide or polyamine [10]. Mathur [11] devel-
decades and has become an integral component of mod- oped a new approach by producing fibrous calcium silicate
ern papermaking. Indeed, for many paper grades mineral hydrates as papermaking fillers. The use of this filler at load-
fillers are the second most important component of the ing levels of 12%-22% was shown to improve sheet bulk, po-
paper stock. Most filled papers are produced for the print- rosity, and light-scattering properties of paper. Yan et al. [12]
ing and writing sector. However, the use of fillers has recently reported that papermaking clay, coated with 2.5%
been expanded recently to package board, newsprint, and starch, provided a 10%-40% increase in tensile index over
tissue [2-4]. Presently, the paper industry uses fillers to control handsheets manufactured solely with clay or clay plus
reduce manufacturing costs, reduce energy consumption, starch added to the papermaking furnish. These studies clear-
and to provide paper products with desired functionality ly document the unique benefits that could be acquired when
and end-use properties. An estimated $2.50 per ton can be starch is directed solely onto the surface of clay particles be-
saved for each 1% increase of filler in paper [5]. Increasing fore papermaking.
the level of filler in paper has become a global interest as This paper reports on our recent laboratory and pilot-scale
a way to: studies directed at evaluating this promising filler technology.
• reduce operating and raw material costs associated with
paper production, EXPERIMENTAL
• increase paper production capacity without adding extra Materials
pulping and drying capacity, and The pulp we used for making handsheets in this study was a
• improve optical and printability properties. commercial unbleached southern softwood kraft linerboard
However, increasing the filler content in paper beyond pulp with a kappa number of 105. Clay fillers with a surface
conventional levels generally results in reduced paper area of 11 m2/g were provided by Imerys (Roswell, Georgia,
strength, increased size demand, abrasion, and dusting. Sev- USA). Raw corn starch B200 was supplied by Grain Process-
eral approaches have been explored to increase filler contents ing Company (Muscatine, Iowa, USA). Raw potato starch was
without detrimentally affecting paper quality, including dif- a commercially available food grade material. Cationic reten-
ferent pulp and filler combinations, preflocculation of filler, tion aid Percol 175 was provided by Ciba (Suffolk, Virginia,
and lumen loading [6-8]. Unfortunately, to date, none of these USA). For the pilot trials, we used reslushed unbleached lin-
technologies have delivered a practical, broadly accepted so- erboard, as described below.
lution for paper manufacturers.
The development of new fillers to improve fiber-filler Filler modification
bonding is an active field of research. Kuboshima [9] has re- We cooked the starch at 95°C for 30 min. In initial handsheet
ported the use of acrylic acid or vinyl acetate to chemically work (Figs. 1-5), the clay was modified by first adding the
march 2008 | TAPPI JOURNAL 
fillers

4. Geometric mean tensile index of calendered SW kraft liner-

board handsheets as a function of clay content with 0%, 2.5%,
and 8.0% corn starch bonded to filler.

1. Ring crush analysis of softwood (SW) kraft linerboard hand-

sheets at varying levels of filler content.

5. ISO brightness of SW kraft linerboard calendered handsheets

as a function of clay content with 0%, 2.5%, and 8.0% corn
starch bonded to filler.

cooked starch, followed by lab drying under vacuum and sub-

sequent grinding to a powder. In later handsheet and pilot
work, we mixed the required cooked starch with clay slurry
at a total solids of 40%-45% for coating, followed by spray dry-
2. Burst index analysis of SW kraft linerboard handsheets at ing of the slurry either at the Institute of Paper Science and
varying levels of filler content employing 2.5% starch bonded to Technology (IPST), Georgia Institute of Technology, in At-
clay filler or starch and clay filler added separately in paper- lanta, Georgia, USA, (anhydrous pilot spray dryer, lab S1, Co-
making process. penhagen) or at Imerys (Figs. 6-11). The mean size of the
particles was determined at IPST with a Malvern System 2600
laser particle sizer.

Handsheet preparation at laboratory scale

Softwood kraft pulp was beaten to 350-400 mL CSF in a Val-
ley beater using standard TAPPI procedures. The pulp was
diluted to 0.40 wt % and targeted amounts of filler were added
before the handsheets were made. After the addition of fibers,
filler, and 1 ppm Percol 175 (based on total slurry solids plus
water) as a retention aid, handsheets were made at a target
basis weight of 180 g/m2 using Formette Dynamique hand-
sheet equipment. The Formette Dynamique was operated at
1.80 bar of spraying pressure and 900 m/min drum speed.
3. Double fold analysis of SW kraft linerboard handsheets at The wet handsheets were pressed at 3.40 bar, dried using a
varying levels of filler content employing clay, 2.5% starch drum dryer (steam pressure 1.36 bar), and then conditioned
bonded to clay filler, or 2.5% starch and clay filler added sepa- at 25.0°C and 50.0% relative humidity overnight.
rately in the papermaking process.

 TAPPI JOURNAL | march 2008

 fillers

6. Tensile index of calendered SW kraft linerboard handsheets

as a function of unmodified clay and spray-dried modified clay.
9. Herty: geometrical mean (GM) of (MD property x CD property)
ring crush vs. clay content.

7. Ring crush of calendered SW kraft linerboard handsheets as

a function of unmodified clay content and modified spray-dried
clay. 10. Herty: bulk vs. clay content.

8. Herty: tensile vs. clay content. 11. Herty: GM stiffness vs. clay content.

width of 0.84 m. Starch-modified clay (1.8% starch applied to

Pilot paper machine conditions clay via spray drying) was added just before the fan pump at
A pilot scale trial was carried out at the Herty Foundation, Sa- targeted levels of 0%, 10%, or 20% clay in the sheet.
vannah, Georgia, USA. Furnish was reslushed liner with a 1:1
softwood-hardwood furnish that was subsequently lightly Determination of handsheet properties
refined to 500-550 mL CSF. The paper machine was operated Paper properties were measured according to standard TAPPI
at 22.8 m/min. Press loads were 4130 MPa (first nip) and 9440 methods. The filler content was analyzed by ashing the paper
MPa (second nip). Headbox consistency was 0.50%. Targeted in a muffle oven according to TAPPI Method T 211 (Ash in wood,
basis weight for the single-ply sheet was 170 g/m2 with a sheet pulp, paper, and paperboard: combustion at 525 degrees C).
march 2008 | TAPPI JOURNAL 
filLers
RESULTS AND DISCUSSION
The benefits of using a starch-coated clay filler with linerboard
were initially evaluated in the laboratory by cooking the starch
in the presence of the filler, drying under vacuum, and milling
the product. The modified clays with 2.5%-5% corn starch
(based on clay) or 2.5%-7.5% potato starch had larger particle
size (about 2-4 µm) than the unmodified clay (< 2 µm). Control
and composite linerboard handsheets were prepared in the
laboratory; Figs. 1-4 summarize the results of physical testing.
The results in Fig. 5 indicate an improvement in brightness
over the no filler control handsheets when the modified 12. Micrographs of Herty sheets: 10% original clay (left) and
starch-coated clay is used. However, these benefits were not 10% modified clay (right).
as dramatic as those associated with unmodified clays, most
likely due to the smaller particle size of the untreated filler.
The results of the laboratory studies demonstrated that as
little as 2.5% starch on clay improved the overall physical per-
formance of the linerboard handsheets. Additional studies
using charged starch derivatives exhibited no significant ben-
efits over underivatized starches.
Although starch-coated clay could be readily prepared in
the laboratory by a cooking-drying-milling process, it was ap-
parent that this was not suitable for large scale production. An
attractive alternative was spray drying. This was accomplished
by mixing a 2.5% charge of precooked corn starch with clay,
which was then spray dried at 20%-40% solids. Following this
approach, the size of the average clay particles increased from
9.52 mm to 38.2 mm, as determined by laser particle sizing; se-
digraph studies yielded comparable results. We evaluated the
13. Effect of clay and modified clay on dewatering.
effect of this change in particle size by preparing softwood
(SW) kraft linerboard TAPPI handsheets with the no clay, un- was made on the Herty No. 1 pilot paper machine at 0.5%
treated clay, and spray-dried clay. These test sheets were sub- headbox consistency. Table I shows the trial plan. It includ-
jected to tensile and ring crush testing (Figs. 6 and 7). These ed a no filler control, liner filled with conventional clay, and
results were comparable to the data reported in Figs. 1-4. liner filled with modified clay.
Samples of the linerboard paper with no clay, unmodified
Herty trial – pilot results with spray-dried clay clay, and spray-dried starch-coated clay were subsequently
To demonstrate the viability of starch coated clays for mill ap- analyzed for physical strength properties. As summarized in
plications, we performed a series of pilot-plant trials at the Figs. 8 and 9, tensile and ring crush increased +10% with the
Herty research facilities. Pilot plant quantities of starch-coated spray-dried modified clay samples over the paper prepared
clay were manufactured using a pilot spray dryer yielding clay from unmodified clay. Bulk and stiffness were equivalent to
particles with 1.8% starch on clay. A single ply liner (170 g/m2) the no filler control for the modified clay at 10% clay content
and retained improved properties over the conven-
Components Control Unmodified Starch-coated clay tional clay at higher loading levels (see Figs. 10 and
(no clay) clay 11). Micrographs indicated larger aggregate size
Filler None 10%; 20% Modified clay (1.8% with the modified clay, consistent with the particle
starch; spray dried@20% size data mentioned above and with the increase in
solids ): 10%; 20%
bulk (Fig. 12). Experimental data also suggested
Furnish Reslushed 1:1 softwood-hardwood commercial liner that the modified clay provided enhanced dewater-
furnish, CSF 500-550 mL ing properties on the table and during pressing; fur-
PM Single ply; BW 170 g/m2 ; 75 feet/min ther studies are needed to verify this conclusion
Chemicals No starch Corn starch (2.5%) Cationic polyacrylamide (Fig. 13).
(pH 6-7) Cationic polyacryl- (Percol 175)
amide (Percol 175) 1 ppm CONCLUSIONS
1 ppm
The development of starch-coated fillers via spray
drying is a viable method to develop innovative
I. Herty pilot-plan papermaking mill trial conditions. bonding clay fillers for real-world linerboard appli-
 TAPPI JOURNAL | march 2008
 fillers
cations. This development is especially attractive because of LITERATURE CITED
its applicability to multiply grades, enhanced paper proper- 1. Gigac, J., Kuna, V., and Schwartz, J., Tappi J. 78(2): 162(1995).
ties, fiber savings, productivity gains, and energy savings. 2. Ozersky, A., Recknagel, R., and Brendle, H.G., “Cellulose-containing fill-
Furthermore, it addresses several of Agenda 2020 Break- ers for paper, tissue, or cardboard products,” PCT Int. Appl. (2006), WO
2006048280 A1 20060511 CAN 144:434695 AN 2006:437077.
through Technology platform challenges [13], including:
3. McLain, L. and Wygant, R., Pulp Paper 80(3): 46(2006).
• Priority 1: Reduced energy in paper dewatering/drying, and
4. Gill, R.A., Haskin, W.J., and Laakso, A-P., “Enhancing the quality of
• Priority 5: Increased filler content with novel material addi- paperboard with precipitated calcium carbonate (PCC) fillers,” PTS-
tive systems that are lower cost than fiber and contribute Symposium 9/1-9/12 (2000).
strength and optical properties equal to or better than fiber. 5. Baker, C. and Nazir, B. in Use of Minerals in Papermaking, Pira
International, Leatherhead, UK, 1988, pp. 83-92.
ACKNOWLEDGEMENTS 6. Green, H.V., Fox, T.J., and Scallan, A.M., Pulp Paper Can. 83(7): 39(1982).
The authors thank the member companies of the Institute of 7. Phipps, J., Paper Tech. 42(7): 37(2001).
Paper Science and Technology, Georgia Institute of Technol- 8. Koizumi, M., Kami Pa Gikyoshi, 42(11): 1022(1988).
ogy, and the Georgia’s Traditional Industries in Pulp and Paper 9. Kuboshima, K., High Performance Paper Soc. 21: 31(1982).
Production (TIP3) Manufacturing Process for their support of 10. Gill, R.A. in Applications of Wet-End Paper Chemistry, (C.O. Au and I.
Thorn, Eds.), Blackie, Glasgow, UK, 1995, pp. 54-75.
this research. Any opinions, findings, conclusions, or recom-
11. Mathur, V.K., “Hydrothermal preparation of xonotlite-foshagite phase
mendations expressed herein are those of the author(s) and calcium silicate hydrates pigments for improved optical and mechani-
do not necessarily reflect the views of GA TIP3. The authors cal properties of papers.” PCT Int. Appl. WO 2001014274 A1 20010301
also wish to thank Z. Yan for his experimental work. CAN 134:182401 AN 2001:152598 (2001).
12. Yan, Z., Liu, Q., Deng, Y., et al., J. Applied Polymer Sci. 97(1): 44(2005).
Received: February 5, 2007 13. Agenda 2020 Technology Alliance, Forest Products Industry Technology
Revised: May 10, 2007 Roadmap, American Forest & Paper Association, Washington, D.C.,
Accepted: August 26, 2007 USA, 2006. Available at http://www.agenda2020.org/PDF/FPI_
Roadmap Final_Aug2006.pdf.

insights from the authors

In setting goals for the industry, AF&PA’s
Agenda 2020 program identified the value
of increasing filler levels in paper and pa-
perboard. In addition, linerboard capacity in
the southeastern United States, especially
Georgia, is intense. It also enjoys a logisti-
cal advantage of being within easy reach of
some of the world’s largest kaolin opera-
tions. Our industrial partners from Georgia
and GA TIP3 recognized these opportuni-
Kim Zhao Patterson Ragauskas
ties and encouraged and supported this re-
search effort.
While other work has shown some im-
provements in strength from using floccu-
lated fillers, the edge crush improvements
in this work are substantially better.
One of the challenges of this work has
been scaling up to an economical level. To
do that we needed to identify an appropri-
ate grade of starch that allowed the solids
to be fed to the spray drier at levels high
enough to make the coat left by evaporat-
ing the water be in a reasonable range.
White Deng Jones Turner
Among the more interesting findings of
this study was that the increase in press director of research at the Institute of Paper Science and
solids is more valuable than just fiber replacement. Of par- Technology (IPST), Atlanta, Georgia, USA; Deng is associate
ticular interest to mills is that every 5% of filler can poten- professor, School of Chemical & Biomolecular Engineering,
tially increase press solids by 1%. Our efforts now will be Georgia Institute of Technology, Atlanta; Jones is director,
to expedite mill usage. Technical Marketing & New Ventures, and Turner is direc-
tor, Business Development, Imerys, Roswell, Georgia; email
Kim and Zhao are research scientists, Patterson is assistant Ragauskas (primary contact author)* at arthur.ragauskas@
professor, Ragauskas is professor, and White is associate ipst.gatech.edu, or Kim at dongho.kim@ipst.gatech.edu.

march
The author has requested enhancement of the downloaded file. All in-text references underlined in blue 2008 | TAPPI
are linked JOURNAL
to publications onResearchG