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Main factors affecting roughening of paper in coating

and printing – A review of recent literature


Xuejun Zou, FPInnovations Paprican, Quebec, Canada

KEYWORDS: Basestock, Coated paper, Coating, calendering, issue for papers containing mechanical pulps, the focus
Fibres, Fountain solution, Mechanical pulp, Printing, of this review will be on wood-containing grades.
Roughening, Roughness, Water absorption
Responses of papers to water application
SUMMARY: Surface roughening occurs when paper is expo- The responses of super calendered (SC) and lightweight
sed to water. This is a typical problem in aqueous coating as coated (LWC) papers to water application in offset prin-
well as in offset printing using fountain solutions. This pheno-
ting are rather different because in SC paper, water is in
menon also occurs in flexography and in water-based gravure
printing. The increasing use of mechanical pulps in many unco-
direct contact with fibres on the surface while in LWC
ated and coated paper grades, coupled with the increasing speed paper, water must penetrate through the coating layer
in coating and printing, has made roughening an important before reaching the fibres. Therefore, SC paper roughens
issue. This report reviews the most recent research findings in significantly more than LWC paper (Chinga et al. 2004,
understanding the phenomenon of roughening and examines the Forseth et al. 1997). As shown in Fig 1, the roughening of
main factors affecting roughening in both coating and printing. SC papers is also accompanied by a significant expan-
Pulp processing and papermaking strategies to minimize roug- sion in thickness, much more than LWC paper.
hening are discussed. Future challenges, opportunities and rese- Pigment coating of mechanical based basestocks can
arch needs are identified. be characterized by a smoothening effect caused by blade
ADDRESS OF THE AUTHOR: Xuejun Zou (xzou@papri-
pressure or by load from the transfer rolls, and roughe-
can.ca): FPInnovations Paprican, 570 Boul. St-Jean, Pointe ning caused by wetting by the coating color. The change
Claire, Quebec, Canada H9R 3J9. in basestock roughness during coating thus depends on
which mechanism is more dominant. For example,
Forseth and Helle reported that for uncalendered
When paper is exposed to water, dimensional changes newsprint, LWC basestock and SC paper (initial PPS
including surface roughening, fibre rising and surface roughness between 6.0 and 8.5 µm), there is no increase
disturbances tend to occur. This is a typical problem in in roughness after coating of paper with “pure water”
aqueous coating as well as in offset printing using followed by drying (Forseth et al. 1997 and 1998). They
fountain solutions. This phenomenon also occurs in flex- suggested that the roughening was compensated by the
ography and in water-based gravure printing. Roughening compression caused by the blade (roughness was actually
during coating causes poor coating layer uniformity and reduced when a sheet was treated with a “dry” blade). For
higher coated paper roughness. On the other hand, calendered papers (newsprint, SC and LWC basestock)
roughening in printing creates poor print quality or even with a roughness ranging from 2.0 to 3.5 µm, water
disrupts the printing. In addition, roughening is application does increase roughness and roughening is
intensified by the high temperature drying, so it is a more dominant (no smoothening by the blade because the
serious issue in heatset web offset (HSWO) printing. paper is already very smooth). The extent of roughening
By definition, surface roughening is the change in the was found to depend on the intensity of calendering, with
roughness of the paper because of the tendency for fibres hard calendering giving low roughening. This indicates
which collapsed during papermaking to return to their that the extent of roughening depends on the initial
uncollapsed state (de-collapsing). Fibre rising is the roughness of the paper as well as its treatment history.
tendency for poorly bonded fibres to rise from the paper Roughening of LWC paper during wetting was obser-
surface. In a study using an environmental scanning ved with an environmental scanning electron microscope
electron microscope (ESEM), De Roever and Cosper (ESEM), first by Forsberg et al. (1992) and then by
showed that fibre rising was a relatively rare event Hallamaa et al. (1999). The water application is achieved
compared to surface roughening (De Roever et al. 1996).
Mechanical pulp is generally regarded as having a greater
roughening potential than kraft pulp (Åslund et al. 2005).
However, it should be pointed out that if heavily
calendered, even wood-free paper roughens when water is
applied (Steffner et al. 1998).
A good review of the literature on this topic was
written by Aspler and Béland (1994). Since then,
however, a large number of papers have been published
with new insights and understanding of the roughening
phenomenon. There is certainly a need to review the new Fig 1. Effect of wetting on paper structure of SC papers – SEM cross-section ima-
information on this topic. Since roughening is mainly an ges (Forseth et al. 1997).

314 Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007
through vapour condensation by lowering the temperature further confirmed by Karnis (1995) who showed that
and increasing the pressure in a chamber. Drying was roughening is affected by the quantity and coarseness of
achieved by returning the temperature to room tempera- long fibre fractions. In a more recent study, Hallamaa et
ture. ESEM surface micrographs of a commercial LWC al. (1997) added different amounts of unrefined and
paper (Fig 2) clearly showed the roughening caused by refined TMP long fibres (rejects) to a GWD-based LWC
the swelling of single fibres under the coating. However basestock, and then tested their roughening tendency
micrographs also showed the re-collapse of raised fibres, using a Prüfbau printability tester and Fibro fibre rising
indicating that the phenomenon is reversible to some tester. Their results showed that roughening of LWC
degree. Ireversible roughening after re-drying was seen in basestock increased significantly with the increasing
those areas with thick-walled fibres. De-collapsing of the amount of unrefined TMP long fibres. However, after
fibre wall was also visible from the ESEM cross-section refining, the negative effect of increasing long fibre
images (Fig 3). This de-collapsing is often also the cause content on roughening is significantly reduced. This was
of coating surface cracks. However, it should be pointed supported by the results obtained by Dooley et al. (2006)
out that the drying used in this study was done at room on calendered newsprint which showed that increasing
temperature and much higher temperature is used in refining energy for long fibres (rejects) reduces the
HSWO printing. High-temperature drying is known to degree to which some fibres recover their original,
intensify the roughening (Ginman et al. 1973, Hoc 1989). uncalendered shape. These results indicate the importan-
ce of refining the long fibre fractions (rejects) to reduce
roughening.
Because coarse mechanical pulp fibres have low
tendency to collapse, it was believed that the walls of
fibres collapsed by calendering have internal
“calendered-in” stresses (Forseth et al. 1997). Water
application reduces the resistance to the calendered-in
Fig 2. ESEM images of a LWC paper surface: a) before wetting, b) during wetting stresses which are then released by the fibre recovering
and c) after wetting. Samples: TMP-based LWC with a coat weight of 8.3 g/m2 its original shape. The thick-walled fibres are believed to
(Hallamaa et al. 1999). have greater calendered-in stresses and, therefore, the
greater potential shape change when stresses are released
stresses (Forseth et al. 1997, Hallamaa et al., 1997).
Forseth et al. (1997) measured the lumens of fibres
present in commercial super calendered papers before
and after calendering and moistening. The results showed
that fibres with the thickest walls had the greatest
roughening response. However, the thick-walled fibres
Fig 3. ESEM images of LWC paper cross-sections: a) before wetting, b) during also showed the greatest response to the roughness
wetting and c) after wetting (Hallamaa et al. 1999).
reduction by calendering. It should be noted that in these
investigations, roughening was studied by exposing paper
Since the moisture can only enter through the surface, the to high relative humidity or soaking in water, which does
change in gloss, when paper is exposed to water, is not correspond to the conditions used in actual pigment
expected to occur first, i.e. before changes in the bulk of coating and HWSO printing.
the sheet. To validate this, Enomae et al. (1997) had Hallamaa et al. (1999) examined the effect of refining
characterized the dynamics of gloss and moisture pick-up TMP rejects on roughening of LWC paper in HSWO
of paper as humidity was increased. Results showed that printing with two oven drying temperatures (130 and
the change in gloss occurs at the same time as the change 165oC). TMP rejects were refined to different fibre coar-
in the bulk as moisture is being picked up. They senesses (from 0.256 to 0.235 and 0.197 mg/m for 14/28
concluded that the changes in gloss results from fraction). Fibre length was kept constant by removing the
cooperative bulk changes: “The surface continues to fines generated during the reject refining. The refined
reflect the reconfiguration of fibres across the sheet even TMP rejects were then added to a GWD and kraft mixtu-
after a long time”. The implication from this study is that re at a constant ratio of 36% GWD, 24% TMP rejects and
in order to stabilize sheet gloss to moisture effect, it may 40% kraft. Results showed that the roughening (the diffe-
not be enough to stabilize the surface only, as is done in rence in roughness before and after printing) is reduced
surface treatment involving a thermal gradient. with refining of TMP rejects when an oven drying tempe-
rature of 165oC is used in HSWO printing (Fig 4).
The role of long coarse fibres in mechanical pulp However, the impact of TMP rejects refining on roughe-
Using a method developed at STFI to evaluate ning at oven drying temperature of 135oC is not signifi-
roughening, Hoc showed that the tendency of fibre rising cant. Much less roughening at both temperatures is
from the surface of handsheets containing mechanical observed when 24% TMP rejects were replaced by kraft
pulp increases with the long fibre content of the pulp. (i.e. 36% GWD and 64% kraft).
Mohlin showed that raised fibres were predominantly Dickson (2001) examined the detailed cross-sectional
thick-walled latewood fibres (Mohlin, 1989). This was changes of a single TMP fibre after calendering and

Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007 315
of stiff and opacifying fines material, causing reduc-
tion in opacity. Most recent studies found that the
alkali peroxide treatment or high-pressure alkali oxy-
gen treatment of TMP rejects reduces fibre coarse-
ness, induces fibre collapse and increases inter-fibre
bonding (Gibbs 2006a and 2006b, Gibbs et al. 2006,
Bian et al. 2007). Tchepel et al. (2006) attributed this
to the reduction in the fibre cross-sectional dimen-
sions which makes the fibre more flexible. This gene-
rates a positive effect on roughening. Gibbs and Allen
found that high-pressure chemical treatment with
alkali and oxygen is much more effective in inducing
fibre collapse than sulfonation treatment (Gibbs et al.
Fig 4. Increase in roughness of LWC paper during HSWO printing (Hallamaa et al. 2006). It should be pointed out that chemical treat-
1999).
ment can may results in a small yield loss (5%).
moistening using confocal laser scanning microscopy
(CLSM). He found that roughening is related to the
amount of fibre collapse during calendering, rather than · Intensive pre-calendering (e.g. using soft-nip calende-
ring with high temperature and moisturizing):
to the wall thickness per se. In a further study by Dickson Unpublished work from Paprican showed that increa-
et al. (2005), mature-earlywood TMP fibres (Pinus radia- sing both calendering load and temperature help col-
ta), with their large perimeters and thick walls, were lapse thick-walled fibres, thus giving better coating
identified as being the most likely to de-collapse during coverage in film press coating (Zou 2005). Yuan and
wetting. Norman et al. (2003) also found that TMP fibres Heitner showed that for coarse TMP pulp made from
from transition wood, with a large diameter and thick Lobblly pine, intensive pre-calendering is the key to
fibre wall is strong enough to de-collapse when exposed preparing basestock for achieving a good coating
to moisture, causing significant roughening. On the other coverage and high coated smoothness (Yuan et al.
hand, although latewood TMP fibres also have thick 2007). This suggested that basestock roughness under
walls and high coarseness, they do not de-collapse as the coating does not spring back to the level before
readily as earlywood TMP fibres after wetting because pre-calendering.
they have small perimeters (Dickson et al. 2005, Norman
et al. 2003). These recent results suggest that not all long Effect of shives
coarse fibres will cause roughening problems. Rather a Kartovaara pointed out that a shive content acceptable for
small amount of shives and thick-walled fibres with a newsprint would be excessive for an LWC basestock, due
large perimeter (mostly from softwood) are the main to sheet roughening originating from the shives
problem. Cleaners are preferred to remove a small (Kartovaara 1990). This is confirmed by SEM cross-
amount of such stiff, poorly bonded thick-walled fibres section images of a LWC paper printed with HWSO
since screens can remove even those long fibres which press. The LWC basestock was made from GWD and
possess adequate bonding ability. Recent research in the kraft. As can be seen in Figs 5(a) and 5(b), the shives in
mechanical pulping area has shown that the large, thick- GWD, whether they are on basestock surface or inside
walled fibres in TMP rejects can be treated with different the basestock, can cause roughening (spring back) in
approaches to create irreversible collapse, thus printing. In this case, the coarse mechanical fibres behind
minimizing their roughening potential. These approaches the coating do not seem to cause significant roughening
include: problems and they de-collapse only partially (Fig 5c).

· Refining of rejects after pre-heating at high


temperature, e.g. 175oC, which is well above the
Roughening tendency of different mechanical pulps
(GWD and PGW vs. TMP and CTMP/BCTMP)
softening temperature of lignin. Norgren et al. (2005) Since TMP (or CTMP) has a larger amount of long and
found that compared to conventional reject refining, coarse fibres than GWD or pressurized GWD (PGW), it
the use of high-temperature creates a higher degree of has been generally thought to have a higher risk of
fibre collapse, particularly irreversible collapse (i.e. roughening during water application (Forseth et al. 1997,
no de-collapse even after re-wetting and drying). This Gane et al. 1991, Liimatainen 1998). Gane et al. (1991)
leads to a higher smoothness and less roughening. reported that with 100% TMP, the basestock beneath the
coating was rougher than prior to coating. Replacing
· Refining of rejects after chemical treatments inclu-
ding sulfonation, peroxide and alkali treatments.
TMP with pressurized GWD resulted in a more stable
basestock which was smoother than it had been prior to
Winberg et al. (1990) found that a high degree of sul- coating, as calculated from the surface profiles of the
fonation of TMP rejects may reduce roughening due basestock before coating and of the coated sheets. The
to improved fibre flexibility and bonding ability, and fact that the basestock beneath the coating layer was
increase sheet smoothness. However, it should be cau- smoother than prior to the coating was attributed to the
tioned that sulfonation treatment reduces the amount compression effect caused by the blade tip.

316 Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007
fibres in BCTMP. However, the effect of BCTMP substi-
tution on roughening in printing has not been studied.

Effect of fines
In an early study, Hoc showed that fines in mechanical
help reduce roughening (Hoc 1989). In a more detailed
study, Forseth et al. (1997) examined the surface
roughening of handsheets made from coarse fibres
(14/28 fraction) with varying amounts of mechanical
pulp fines (from 0 to 28%). They found that increased
fines content in paper improves smoothness before and
after calendering and the effect remains even after
moistening the calendered paper. Roughness after
moistening does not go back to the original roughness, as
shown in Fig 6. This shows that mechanical pulp fines
per se do not decrease roughening, but give lower rough-
ness to start with (also due to the reduced proportion of
coarse fibres).

Fig 5. SEM cross-section images of a GWD-based LWC paper after HSWO printing
(Zou, 2005).

Significant advances in mechanical pulping in recent


years have made it possible to produce TMP or CTMP
more suitable for printing and coating. Ahlroos et al.
(2001) found that although significant roughening takes
place for both types of papers, there is little difference in Fig 6. Effect of fines content on roughness of handsheets before and after calen-
dering and moistening (moistening was done by exposure to humid air at 97% RH
roughening (as measured by PPS roughness increase)
for 24 hours) (Forseth et al. 1997).
between film-coated GWD and TMP based LWC paper
in HSWO printing. Hallamaa et al. (1999) found that
partially replacing GWD with unrefined TMP rejects Effect of filler content
slightly increased roughening. However, replacement Increasing filler content is believed to cause more
with refined TMP rejects did not increase roughening in roughening during water application because it reduces
HSWO printing. This indicates that the difference in fibre to fibre bonding (Aspler 1994, Forseth et al. 1997).
roughening tendency between GWD and TMP depends On the other hand, increasing filler content can reduce
on how TMP is produced. Many factors including pulp the pore volume which leads to decreased water
freeness, reject refining, post-refining, use of pre-calen- penetration. Ahlroos et al. found that increasing filler
dering, and coating methods affect the roughening content (from 10% to 20%) reduced the roughness of
tendency of final coated paper. Roughening of TMP- LWC basestock and the reduction in roughness was
based LWC papers can be minimized if TMP is appropri- preserved even after coating, indicating that increasing
ately processed (e.g. good cleaning, screening and reject filler content does not increase roughening in coating
refining) and if intensive pre-calendering is used (Zou et applications (1998 and 2001). Higher filler content in
al. 2002). basestock has also resulted in slightly less roughening in
The effect of substituting kraft with BCTMP in wood- HWSO printing (Hu et al. 2007).
free coated paper was studied by Hu et al. (2006 and Reme et al. (2003) used stereo SEM cross-section
2007). They found that at a substitution level lower than imaging to examine the changes in micro-roughness of
20%, BCTMP does not cause a significant increase in SC papers during moisturizing in a Prüfbau laboratory
roughness of the coated sheets, indicating that printing press (this SC paper contained 35% filler, 10%
roughening is not significant during coating. However, at kraft, 10% GWD and 45% TMP, with a grammage of 56
a higher BCTMP substitution level (>20%), a higher g/m2). They observed that on the areas containing mecha-
roughness and lower gloss were found, indicating the nical pulp fibres on the surface, micro-roughness, measu-
tendency of roughening caused by BCTMP. A high red as surface height standard deviation, increased by 0.8
calendering load is needed to achieve the roughness and µm while areas covered with fines and fillers roughened
gloss targets similar to those without BCTMP. The incre- less, with an increase of only 0.35 µm.
ased roughness was attributed to the presence of coarse

Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007 317
Effect of wet pressing blished that the roughening tendency of paper depends
There is not much research in the literature specifically strongly on the extent of calendering and highly calende-
focusing on the effect of pressing on surface roughening. red papers tend to have a large increase in roughness
In a laboratory study using handsheets, Skowronski upon wetting. Early work by Skowronski (1990) showed
found that press-dried sheets (using a Wabash hydraulic that most of the improvement in smoothness by calende-
press at 177oC at two different pressures of 0.41 MPa and ring (with a hard nip at 48 kN/m and 50oC is lost after
3.45 MPa for 30 seconds) had the same extent of roughe- wetting. Gane et al. (1989) as well as Engström et al.
ning as the wet-pressed sheets with air drying (1992 and1994) obtained similar results showing that the
(Skowronski 1990). Sasaki et al. (2000) found that the roughness of uncalenedered basestock was not affected
roughening of a press-dried TMP sheet was much lower by coating, but all the smoothening effects of pre-
than that of calendered TMP sheets. Since wet pressing calendering was lost during coating, i.e. the roughness
generally increases the interfibre bonding, it is expected beneath the coating was the same for uncalendered and
to have some positive effect in decreasing roughening in pre-calendered basestocks. Fibre flocs that are compres-
both coating and printing. This is speculated to be due to sed by pre-calendering were found to “pop up” more
hornification of the fibre walls caused by heat and when exposed to the aqueous phase in the coating colour
pressure (Sasaki et al. 2000). In addition, intensive (Engström et al. 1992 and 1994, Retulainen 1997). More
pressing may also help permanently collapse mechanical recent work, however, has shown that the smoothening
pulp fibres, similar to the effect of pre-calendering. effect achieved by calendering or pre-calendering is
However, it should be pointed out that in practice, most partially preserved (Forseth 1998, Steffner et al. 1998,
of the mills operate their pressing section at maximum Zou 2005, Yuan et al. 2007). The different observations
loadings so not much flexibility exists. here may be due to the intensities (temperature and load)
of pre-calendering, furnish type, as well as testing and
Effect of hydrophobic sizing characterization methods (indirect vs. direct).
A study by LePoutre et al. (1986) showed that hydro- Thermal gradient (TG) calendering (hard nip, 49 kN/m
phobic sizing had no effect on roughening of LWC bases- and 203oC) was found to produce paper with lower
tock. Hydrophobic sizing (AKD size) was applied from roughening tendency during coating (Skowronski 1990,
hexane solution to maintain the sheet structure. In a Skowronski et al. 1990). In a following study using
similar study, Forseth et al. (1998) found that water- “water coating”, i.e. applying pure water rather than real
induced roughening of pre-calendered newsprint was coating colour, Forseth et al. (1998) found that although
reduced by increasing hydrophobic sizing, but the there is some roughening with wetting, part of the
reduction was small compared to the overall moisture- smoothening effect by pre-calendering (soft-nip) on
induced roughening. For uncalendered newsprint, no wood-containing papers is retained after wetting and re-
such effect was found. Blohm et al. (2001) found that drying. Furthermore, it was found that higher intensity
surface sizing has no effect of roughening tendency of pre-calendering (150 kN/m, 90oC) gives less increase in
pre-calendered wood-free basestock during coating. roughness than mild calendering (120 kN/m, 60oC).
These findings may be explained by the following Steffner et al. (1998) found that soft-nip calendering
mechanisms: gives less roughening tendency than hard-nip calende-
ring. Dooley et al. (2006) found that at the same linear
· Hydrophobic sizing can stop bulk water absorption
but has no effect on vapour phase diffusion into inter-
load, increasing calendering roll temperature reduces
roughening tendency. This can be explained by two
fibre pores or molecular diffusion into fibre walls. mechanisms:

· Significant external pressure is placed on paper under


a blade or at the printing nip when coating or water is
· Crushing of fibres due to intensive pre-calendering.

applied. In this situation, the impact of surface che-


mistry on water penetration is significantly less.
· Thermoplastic softening of the lignin in fibre wall
due to the increased calendering temperature.

These results indicate that hydrophobic sizing of Recent work on film press coating has showed that
basestock is not an effective way of reducing roughening. pre-calendering improves coat weight uniformity and
coated papers smoothness (ahlroos et al. 1998). Results
Effect of calendering and pre-calendering from Paprican support this (Zou 2005). In a pilot trial, a
Calendering is used to achieve the high smoothness LWC basestock (39 g/m2) made from 70% softwood
required for printing for newsprint and SC papers while CTMP and 30% kraft was pre-calendered using both
pre-calendering is used to prepare the basestock for hard-nip and soft-nip calendering and then coated.
lightweight coating. Calendering or pre-calendering can Roughness of the basestock before and after coating was
significantly reduce roughness, but it also has a measured using image analyses of the SEM cross-section
significant effect on the roughening tendency during images. The results in Table 1 show that although rough-
coating and printing (Gane et al. 1989, Skowronski 1990, ness increases more after coating for the pre-calendered
Skowronski et al. 1990, Engström et al. 1994, Retulainen basestocks, it is still much lower than for uncalendered
1997, Forseth 1998, Steffner et al. 1998). It is well esta- basestock. As can be seen from the cross-section images

318 Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007
Table 1. Effect of different calendering conditions on roughness of a 38.5 g/m2 basestock
before and after coating (Zou 2005).

Properties No pre- Hard nip Low intensity High intensity


calendering (50 kN/m 96oC) soft-nip soft-nip
(200 kN/m,100 C) (250 kN/m,175oC)
o

Caliper (µm) 87.6 65.2 59.2 53.5


Roughness
before coating (µm) 8.9 5.3 4.0 3.0
Roughness under 7.5 6.0 5.0 4.6
coating (µm)
Coating thickness 71.0 65.1 58.0 50.9
variation (COV, %)

in Fig 7, the thick-walled TMP pulp fibres (softwood)


collapsed by pre-calendering did not completely de-col- Fig 7. SEM cross-section images of coated papers (Zou 2005).
lapse (or recover) after coating. Compared to uncalende-
red basestock, pre-calendered basestock gave a better Table 2. Pre-calendering concept for LWC papers (Banecki et al. 2004).
coating coverage, and also a smoother coated surface.
This indicates that although pre-calendered basestock Concept Conventional pre-calendering Reinforced pre-calendering
(1-nip hard nip) (2-nip soft nip)
does roughen more during coating application, it is still
Surface temperature <120oC ≤200oC
effective in improving coated paper smoothness and coat
Linear load <60 kN/m ≤250 kN/m
weight uniformity. Soft-nip calendering with a high tem-
Web moisturizing No Yes, on both sides
perature was found to be better than hard-nip because it
helps collapse the thick-walled fibres on the surface
while maintaining a high bulk. pre-calendering. In another study, Ahlroos et al. (2001)
The somewhat different effects of pre-calendering on found that pre-calendering has no significant effect on
roughening observed between film press and blade coa- roughening of TMP-based LWC paper, but pre-
ting may be due to the following factors: calendering still gives a slightly higher print smoothness
(due to a lower coated paper roughness).
· There is no contact between basestock and coating
before application in metered size press coating, Effect of coating formulations and dewatering
while there is always some distance between the Since roughening during coating applications is caused
applicator and blade. by the penetration of water from coating color into
basestock, the properties of coating color such as solids
· The pressure at the film transfer nip is lower than the
pressure pulse under blade, and this may result in less
content, viscosity, water retention are expected to affect
roughening. By comparing the surface profile of the
water penetration. basestock before coating with that of the coated surface,
Gane et al. (1989) observed different roughening
Because high-temperature pre-calendering helps pro- tendency when coating formulations with fine and coarse
duce a more closed and smoother surface for coating and clay pigments were used. This was attributed to their
has no negative effect on roughening during film press difference in dewatering characteristics. A rapid
coating, it has become an important part of newly dewatering, loosely packed pigment (coarse clay)
installed LWC machines using film press coating immobilizes rapidly and limits the extent of surface
(Banecki et al. 2004). The use of pre-calendering makes relaxation of the basestock such that any induced
it possible to use TMP or CTMP in LWC grades. To roughening is virtually independent of coat weight and
reach the quality requirements placed on both LWC rate of drying. A slow dewatering closely packed pigment
rotogravure and HSWO printing paper using film (fine clay) induces a varied amount of roughening,
coating, reinforced pre-calendering that utilizes both depending on coat weights. At high coat weight the effect
moisture and temperature gradient calendering is is greatest, but at low coat weight, under conditions of
proposed as shown in Table 2. Higher linear load and rapid drying, roughening is minimized (Gane et al.
surface temperature are used than those in a conventional 1989). These results indicate that in blade coating,
hard-nip pre-calendering. The reinforced pre-calendering roughening may also depend on the type of applicator
may also help permanently collapse the large, thick- (e.g. short dwell, long dwell, and roll applicators)
walled mechanical pulp fibres (see Fig 7). Hard-nip because of the difference in contact time between
calendering could not be used at the same loading level application and meeting.
as soft-nip calendering because the basestock strength In HSWO printing, roughening occurs only when the
would be reduced to unacceptable levels. basestock is in direct contact with water in fountain solu-
In terms of roughening in HSWO printing, the results tion or water-emulsified ink. Therefore, a coating layer
obtained by Ahlroos et al. on a GWD-based LWC paper structure which controls the transfer and absorption of
showed that pre-calendering reduced roughening (1998). water is expected to have a significant effect on roughe-
This was attributed to the improved coating coverage by ning. In a laboratory study using an ESEM, Grön et al.

Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007 319
(1996 and 1998) observed that clay-based coating had
less roughening than pure GCC coating. Roughening of
coated paper with a mixture of clay and GCC was similar
to that of pure clay coating. They stated that the pigment
choice has a significant effect on surface roughening.
They also found that molar mass density and amount of
CMC has some effect on surface roughening. Adding
CMC (up to 0.7 part per hundred parts of pigment) or
using higher molar mass CMC reduced roughening. The
influence of CMC was greater for clay-based coating
Fig 8. Effect of moisture level on printed smoothness and gloss (Ewens et al.
possibly due to the stronger association between CMC 2003).
and clay and the large contact area between clay
pigments. GCC appears to be more sensitive to surface tact with water and thus have a higher risk of roughening.
wetting because of the low contact area between pigment Chinga et al. (2004) also observed some small diffe-
particles resulting from rhombic shape of the particles. rences in roughening between blade and film-coated
An additional explanation for the water sensitivity of the LWC papers, with blade coated paper having a slightly
GCC coating is that CMC does not interact or associate higher roughening tendency. They speculated that there
to any extent with GCC. (Grön et al.1996 and1998). were more “protruding” fibres on the surface of blade
In a more recent study at KCL, Tuominen et al. (2003) coated paper because it contained large amounts of TMP
found that there is less fountain solution transferred to (the film-coated paper contains GWD and de-inked
clay coating than GCC coating. As a result, significantly pulp). Because of the different furnish used in their study,
less water was absorbed by clay coating, as indicated by a the difference in roughening cannot be attributed solely
smaller hygroexpansion of paper. The higher tortuosity of to the difference in coating methods. It should be pointed
clay coating may also prevent the penetration of fountain out that at typical coat weight of 9-10 g/m2, the difference
solution into the basestock. In addition, they found that in coating layer uniformity between blade and film coa-
hydrophobic treatment of pigments (GCC and clay) has ting is rather small and occurs mainly at the scale of a
no effect on the amount of fountain solution transferred, few hundred microns [36]. Since the advantage in coating
but reduced fountain solution penetration into the GCC layer uniformity for film press coating over blade coating
coated paper (but no significant effect on clay coated is at lower coat weights (< 9 g/m2) (Grön et al. 1999), the
paper was found). This may be explained by the fact that positive effect of film press coating on roughening in
fountain solution transfer is affected by nip pressure, and HSWO printing should be more pronounced at lower coat
the following penetration is slowed down by hydrophobic weights.
sizing. In the case of clay coating, low fountain solution
transfer and high tortuosity reduced the effect of hydro- Effect of moisture content of paper before printing
phobic sizing. Since roughening by water application is Ewens et al. (2003) found that if a lightweight coated
always accompanied by paper expansion, a similar effect sheet is dried to low moisture content (<4%) during
of coating pigments is expected on roughening, that clay super-calendering, less surface roughening occurs, as
coating could have less roughening tendency in HSWO indicated by better print gloss and better printed smooth-
printing. ness (Fig 8). This may be due to the fact that each time a
It should be cautioned that adding hydrophobic sizing sheet is dried, the fibre saturation point and water
chemical in coating colour may reduce surface strength diffusivity into the fibres are reduced (Scallan 1992). In
(adhesion among pigments and between coating and fact, some “self-sizing” effect when sheet moisture level
basestock), leading to piling during HSWO printing. is reduced to 3% or less, and this was believed to reduce
More detailed research is certainly required on the effect the rate of water penetration (Ewens et al. 2003). As a
of coating formulations on roughening, particularly on result, water induced fibre swelling is then reduced in
changing pigment size and size distribution as well as offset printing, resulting in reduced roughening. The
blending of different pigments because they have a signi- improved print gloss results in part from the
ficant impact on coating structures (Vidal et al. 2004, improvement of printed smoothness, as well as reduced
Larsson et al. 2005). ink-setting rate.

Effect of coating methods Effect of water and fountain solution absorption


The film coating technique gives a sheet a lower roughe- For papers made of mechanical pulps, Åsland et al.
ning tendency during the coating stage and also in (2005) found a linear relationship between the increase in
HSWO printing than blade coating (Ahlroos et al. 1998, roughness and the amount of water taken up by paper.
Banecki et al. 2004). Less roughening in coating is due to This shows that water absorption by paper in coating or
pre-metering of wet coating film and shorter contact time printing affects roughening. On the other hand, the majo-
between wet coating and basestock. On the other hand, rity of previous studies on roughening have been done
less roughening of film coated papers in HSWO printing with pure water. This is relevant to coating. However, in
was attributed to more uniform coating layer (Gane et al. offset printing, a fountain solution rather than pure water
1998). Lower coat weight area can be more easily in con- is used. Since a fountain solution is quite different from

320 Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007
pure water in terms of surface tension [59], its rate of al. Above its Tg, it behaves as a viscoelastic material, and
penetration into paper or coating may be very different, can deform and flow. Since water acts as a plasticizer, the
thus causing different degrees of roughening. In addition, Tg declines quickly with humidity and is below room
the acidic nature of the fountain solution may cause temperature at 50% RH.
damages on calcium carbonate based coatings, thus Lignin, the remaining 20-30%, is a cross-linked three-
affecting roughening of coated papers. Therefore, more dimensional polymer, with amorphous regions between
research using fountain solution is needed. the cross-links (Alén 2000, Koch 2006). Native lignin has
a Tg of about 100oC (120-130oC after mechanical pulping
Effect of drying in printing treatment). It penetrates intimately the microfibril-hemi-
Although roughening is caused mainly by water applica- cellulose network. Native lignin has none or very few
tion, it can be intensified by heating and drying (Ginman hydrophilic groups. It is not sensitive to water. Like
et al. 1973, Hoc. 1989, Hallamaa et al. 1999). Hallamaa hemicellulose, it behaves as a viscoelastic polymer but
et al. (1999) examined the roughening in a one-colour with high elasticity because of the cross-links.
HWSO printing at two different drying temperatures (130 The native form of a wood fibre is a hollow tube.
and 165oC). Significantly more roughening was observed During papermaking, wet-pressing and surface tension
when a drying temperature of 165oC is used (see Fig 4). forces, during dewatering and drying, exert z-directional
So lowering dryer temperature is beneficial in reducing stresses that may, if the fibre is sufficiently flexible,
roughening. However, this may require operating a prin- collapse partly or totally the hollow tube. The fibre wet
ting press at lower speed which is not always practically flexibility increases quickly with decreasing pulping
possible. yield, as the stiff lignin matrix is attacked or dissolved
(Scallan 1992). In addition, the ratio of wall thickness to
Discussion on the mechanisms of roughening tube diameter is an important parameter controlling wet
Based on the observations described in this review, the flexibility. The diameter depends much on wood species
following mechanisms appear to apply. To fully under- but springwood fibres tend to have thinner walls with
stand these mechanisms, however, one needs to review larger diameters than late summerwood fibres.
the structure and chemistry of wood fibres and how they The fibre saturation point (FSP) of a never-dried wood
influence the mechanical properties. fibre is around 1.3-1.4 g water/g fibre (Scallan 1992). In
The wall of a wood fibre broadly consists of crystalli- other words, the solids content is about 34% (v/v). Since
ne cellulose microfibrils embedded in an amorphous the water is mostly associated with hemicellulose, the lat-
matrix of hemicellulose and lignin. Cellulose microfibrils ter can be visualized as an 8.5% v/v polymer gel. In the
represent approximately 40-50% w/w (Alén 2000, Koch un-delignified fibres, the three-dimensional lignin matrix
2006) and are not sensitive to water because all the OH remains and the fibres have low wet flexibility. In the
groups are tightly tied up to each other in the crystal net- delignified fibre, hemicellulose is now a 15% viscous
work, except a few on the surface. Microfibrils are rigid polymer gel surrounding the cellulose microfibrils. The
and provide stiffness and strength to the fibre (Alén wet fibre is very flexible and deformable. Once dried and
2000, Gruber 2006, Koch 2006, Sixta 2006). Cellulose rewet, the FSP is much lower, typically 1.0 g water /g
chain ends, and chains that may go from one microfibril fibre as some of the inter-chain hydrogen bonds formed
to another through less oriented, non-crystalline regions during drying are resistant to the swelling pressure
are called amorphous cellulose (Alén 2000). Amorphous (Scallan 1992, Alén 2000, Sixta 2006). Shearing stresses
cellulose is sensitive to water because not all hydroxyls during beating help break these bonds and the FSP goes
are tied up into close hydrogen bonds. The microfibrils up, and even may go back to 1.3 g/g on a fully beaten
have different orientations in each layer (or lamellae). kraft fibres (Scallan 1992, Alén 2000, Sixta 2006).
Hemicelluloses (circa 25% w/w, Gruber 2006), due to During dewatering, wet press load and surface tension
their chemical structure, cannot achieve the high order forces tend to collapse the fibres. The hemicellulose gel
and density required for forming crystalline regions and between the microfibrils may flow to conform to the new
are therefore amorphous. When dry, amorphous hemi- configuration. Inter-diffusion of the hemicellulose chain
cellulose polymer chains or chain segments have their segments at the interface between two fibres or between
hydroxyls loosely bonded to one another or free. These the inner walls in the collapsed lumen leads to the
amorphous domains are very sensitive to water. Water formation of strong bonds. The dry delignified fibres
molecules can diffuse to the free hydroxyls and to the remain collapsed into “ribbons” after surface tension
weak hydrogen bonds, breaking them to form stronger forces disappear. In the un-delignified fibres, the lignin
hydrogen bonds than the ones they replace - stronger matrix may prevent flow of the hemicellulose and the
because the water molecule can approach the hydroxyl fibres may simply deform elastically and recover once
closer than the one it replaces and that comes from the forces are released. To the extent that hemicellulose
another polymer chain. As a result, very strong swelling flow took place, the dry fibre may remain uncollapsed,
forces develop (osmotic pressure) when water (liquid or partially collapsed, and even sometimes fully collapsed.
vapor) is present in amorphous cellulose and hemi- Uncalendered paper shows little permanent dimens-
celluloses (Alén 2000, Gruber 2006, Sixta 2006). Dry ional changes upon rewetting and re-drying as related to
hemicellulose has a glass-transition temperature Tg fibre shape recovery. Most permanent dimensional chan-
above 100oC. Below its Tg, it behaves as a brittle materi- ges are due to drying under tension. During calendering,

Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007 321
z-directional stresses force the tube into a ribbon or fur- deformation if the bonds resist the residual unbending
ther flatten ribbons. At the molecular level, bonds bet- stresses when the load is removed. However, upon rewet-
ween adjacent hemicellulose chains may break under the ting, water diffuses to the bonding sites and may break
load, and some permanent polymer flow may occur in the the bonds, in which case the unbending stresses return
hemicellulose-lignin domain with formation of new the fibres or shives back into their uncollapsed shape.
bonds. Once the load is released, any elastic deformation Water may also create swelling stresses that combine
is released immediately There are now two possibilities: with the unbending stresses to break the bonds. Upon
The fibre returns elastically to a configuration correspon- drying, however, the fibres or shives will remain uncol-
ding to the extent of permanent flow; or it may remain lapsed: The “de-collapsing” of shives is irreversible.
deformed (flattened) if new bonds have developed bet- The changes in fibre dimension and shape with calen-
ween adjacent hemicellulose chains. Therefore, an inter- dering, water application and drying are illustrated in
nal stress is then built into the fibre. The new bonds bet- Figs 9 and 10. Based on these mechanisms, several gene-
ween hydroxyls on adjacent hemicellulose chains are ral pulping and papermaking strategies may be used to
however, as was explained earlier, less stable than those reduce roughening:
between hydroxyls and water molecules so that they will
break in the presence of moisture and the fibre will reco-
ver, elastically, to an uncollapsed shape, aided by the · Introduce chemical groups that will make the lignin
less hydrophobic and more swollen (chemi-mechani-
swelling forces. Upon re-drying, the fibre will not collap- cal pulp).
se: Shape recovery to a tube is irreversible. By contrast,
delignified fibres, once contacted with water will swell
strongly but recover their collapsed configuration once · Plasticize the fibres and shives by loosening their
structure mechanically through refining/beating so
re-dried. Swelling is reversible for delignified fibres.
Within the range of un-delignified to fully delignified
fibres currently available for papermaking, the behavior
· that they will be less resistant to de-collapsing during
drying.

may range between the two extremes described. Collapse the fibres when they are still plasticized by
The balance of viscous to elastic deformation will
depend on the water content and the temperature at the · water (e.g. wet-pressing or refining).

time the load is applied, as well as on the history of the


pulp fibre. In turn, moisture and/or temperature can be
used to ensure that there is as little as possible elastic
· Use heat to soften the lignin while pressing or hot-
calendering.

deformation under the load. Hot calendering in the


presence of added moisture uses this approach. Intense
wet pressing or, better, press-drying are other methods.
The other approach is to promote swelling of the ligni-
fied fibres by mechanically breaking hydrogen bonds in
the hemicellulose matrix, through refining, in order to
help polymer flow and maximize the amount of perma-
nent collapse during drying and to minimize the extent of
elastic deformation.
Structural changes in the sheet are enhanced by the
breaking of inter-fibre bonds when water diffuses in the
hemicellulosic inter-phase between fibres releasing any
residual stresses. Upon drying, “never-dried” chemical
pulp fibres which are plasticized by water collapse into Fig 9. Response of kraft and mechanical fibres to water application.
ribbons under the effect of capillary forces. They may
need a little bit of refining (beating) if they are not
“never-dried”. Upon rewetting, they will swell, and may
return to their uncollapsed state. However, upon re-
drying, they will again collapse. Calendering does little
further collapse but may induce a few residual stresses.
Upon rewetting, water diffuses into the fibre walls,
swelling occurs, but is almost totally reversible upon re-
drying.
Mechanical pulp fibres or shives show little or no
collapse during drying, particularly if they are thick-
walled. Lignin is below its glass transition temperature
and resists deformation by the capillary forces. During
calendering, surfaces are pressed into contact and bonds
(intra- or inter-fibre, mostly Van der Waals, and hydrogen Fig 10. Response of thick-walled mechanical fibres to calendering and water
bonds) may form. This may result in a “permanent” application.

322 Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007
Conclusions
reducing roughening. To better utilize the thick-walled
A significant amount of research results from recent stu- fibres, chemical and thermal treatment to plasticize the
dies has shown or confirmed that: fibre wall, combined with post-refining, should be the
focus of research to make fibre swelling more reversible.
· Roughening is caused mainly by irreversible de-col-
lapsing of fibres when in contact with water.
Fountain solution is quite different from pure water, with
an acidic pH and a wide range of surface tensions.
Therefore, there is a need to examine the impact of
· Roughening process involves fibre swelling, bond
breaking and release of internal stresses as a result of
fountain solution type and properties on roughening of
paper, particularly coated papers.
the molecular diffusion of water into fibre walls. New coating technologies such as spraying and curtain
coating have emerged as potential alternatives to blade
· Key fibre properties that affect roughening are fibre-
wall thickness, perimeter and collapsibility. Thick-
and film press coating. How they affect water-paper
interactions and roughening during coating is not clear.
walled fibres do not always de-collapse during re- Because of their claimed better coating uniformity, they
wetting and drying because the de-collapsing is also may have some positive effect on roughening in printing.
affected by the perimeter, as well as the extent of per- However, more research is needed to confirm this.
manent collapse by calendering. The key factors controlling roughening include fibre
properties (perimeter, wall thickness, swelling ability),
· Coarse softwood TMP or CTMP, if processed proper-
ly, can have similar or even less roughening than
the amount of stress built into the fibres and sheet, and
amount of water absorbed by fibres. It would be very
GWD in both coating and printing. Refining of useful to develop a quantitative relationship linking roug-
rejects using more energy, high temperature and che- hening to these factors.
mical pre-treatments to increase fibre collapsibility is
important. Acknowledgement:

· Although part of roughness reduction by pre-calende-


ring is lost during water application, it is still effective
The author would like to thank Dr. Pierre LePoutre of FPInnovations Paprican for
the critical comments and insights into the mechanism of roughening.
in achieving better smoothness and coverage particu-
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Hu, K., Ni, Y., Zhou, Y. and Zou, X. (2006): Substitution of Hardwood Kraft with Zou, X., Vidal, D. and Allem, R. (2002): Film Press Coating: Coated Paper Quality
Aspen High Yield Pulps. Part I. Synergy on Basestock Properties, Tappi J. 5(4), and Basestock Effects, Proceedings of the TAPPI Metered Size Press Forum III,
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Karnis, A. (1995): Effect of Wood Species and Process on the Linting Propensity Accepted March 29, 2007

324 Nordic Pulp and Paper Research Journal Vol 22 no. 3/2007

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