全 文 ：第 51 卷 第 3 期
2 0 1 5 年 3 月
林 业 科 学
SCIENTIA SILVAE SINICAE
Vol. 51，No. 3
Mar．，2 0 1 5
doi: 10．11707 / j．1001-7488．20150315
Ｒeceived date: 2014 － 05 － 06; Ｒevised date: 2014 － 11 － 05．
Foundation project: National Nonprofit Institute Ｒesearch Grant of CAF(CAFINT2012C02) ．
装饰原纸用自乳化苯乙烯丙烯酸酯表面
处理剂的制备及表征
徐建峰 龙 玲 于家豪
(中国林业科学研究院林业新技术研究所 北京 100091)
摘 要: 【目的】采用乳液聚合法，制备一种自乳化苯乙烯丙烯酸酯( SAE)表面处理剂。在苯乙烯丙烯酸酯乳
液的制备过程中，引入带有亲水性羧基的丙烯酸作为乳化剂，丙烯酸既与其他单体发生交联反应，赋予最终产品
良好的机械强度，其羧基的存在又赋予最终产品一定的亲水性。这样既可保证传统表面处理对装饰原纸纸张性
能、尤其是关键参数适印性的提高，又能保持装饰原纸的吸收性。【方法】采用苯乙烯 ( St)、丙烯酸丁酯 ( BA)、
甲基丙烯酸甲酯(MMA)为主要单体，引入丙烯酸 (AA)为功能单体，制备自乳化型苯乙烯丙烯酸酯乳液用作装
饰原纸表面处理剂，考察丙烯酸用量、引发剂用量以及硬、软单体质量比对乳液性能及表面处理效果的影响，使
用扫描电子显微镜( SEM)、显微红外光谱仪、激光粒度仪、旋转黏度计、电荷密度测试仪等对所制乳液进行表征。
【结果】当丙烯酸用量为 8wt%、引发剂(过硫酸铵)用量为 0. 3%、mSt /mBA 为 1. 5 ∶ 1时，所制乳液性能优良，乳液
粒径 130 nm 左右，黏度 20 mPa·s，电荷密度 0. 7 mmol·L － 1。装饰原纸经所制乳液配制表面处理剂处理后，纸页
表面形成一层膜，且有羧基存在; 在吸收性保持的前提下，装饰原纸的适印性显著改善。【结论】引入带有亲水
性、反应性羧基的丙烯酸作为功能单体制备苯乙烯丙烯酸酯类装饰原纸表面处理剂，有别于传统的表面处理剂，
同时解决了提高装饰原纸表面性能、适印性，且保证装饰原纸吸收性两大难题，是改善装饰原纸产品品质的一种
有效的方法。
关键词: 自乳化苯乙烯丙烯酸酯; 装饰原纸; 表面处理; 适印性; 吸收性
中图分类号:TS69 文献标识码:A 文章编号:1001 － 7488(2015)03 － 0116 － 08
Preparation and Characterization of Self-Emulsifying Styrene Acrylate
Emulsion Used as Surface-Treatment Agent for Decorative Base Paper
Xu Jianfeng Long Ling Yu Jiahao
(Ｒesearch Institute of Forestry New Technology，CAF Beijing 100091)
Abstract: 【Objective】Decorative paper，which was widely used in the surface finishing of wood-based panels，can not
only protect the wood-based panels from wear，heat and contaminations，but also endow the products with excellent visual
effects． With the development of wood-based panel industry and the related fields，more and more attention has been paid
to the properties of decorative paper，which are determined by the properties of the decorative base paper directly． Among
the performance indices of decorative base paper，the two key indices are printability and absorbability． The former affects
the print quality and the latter affects the absorption of melamine in the production of decorative paper． In general，surface
treatment is considered as an effective method to obtain excellent printability of decorative base paper， but weak
absorbability of paper is also found in traditional manufacturing method． Thus，new types of surface-treatment agents are
needed to develop．【Method】Styrene ( St)，butyl acrylate ( BA )，methyl methacrylate ( MMA ) were used as raw
materials． Acrylic acid (AA) was introduced as the functional monomer． The latex was used in the surface-treatment of
decorative base paper for good printability and absorbability． The influencing factors，such as the dosage of acrylic acid，
the dosage of initiator，the mass ratio of hard monomer with soft monomer，were studied and the optimal conditions were
achieved． Then，the products were characterized by scanning electron microscopy，microscopic infrared spectroscopy，
laser particle size analysis，rotational viscometer and particle charge detection．【Ｒesult】The results showed that the
第 3 期 徐建峰等: 装饰原纸用自乳化苯乙烯丙烯酸酯表面处理剂的制备及表征
excellent performance and good surface-treatment effect of self-emulsifying SAE were achieved when the reaction conditions
were controlled as follows: 8wt% AA，0． 3wt% ammonium persulfate，mass ratio of styrene (St) to butyl acrylate (BA)
1． 5:1． Under the optimal conditions，the latex particle size was around 130 nm． The latex viscosity was 20 mPa·s and
the latex charge density was 0． 7 mmol·L － 1 ． Compared with untreated paper，the printability of the decorative base paper
was apparently improved and the absorbability of paper sheet was maintained． When the coating weight was 2 g·m － 2，the
capillary rise was 19 mm·(10min) － 1 ． The surface strength was 1． 1 m·s － 1 and the smoothness was 130s，which were
better than the values of national standard GB /T 24989—2010． The surface-treated paper was covered by film partially
and carboxyl was observed on the paper．【Conclusion】When acrylic acid，which has hydrophilic and reactive carboxyl，is
introduced as the functional monomer for the preparation of SAE，the self-made surface treatment agent can simultaneously
meet two demands: improving the surface property and printability of paper，and maintaining the absorbability of paper．
Introducing self-emulsifying styrene acrylate emulsion as surface-treatment agent is an effective method for improving the
quality of decorative base paper． In the future study，the type，dosage and adding method of functional monomer，and the
same role as AA in this paper，should be researched emphatically．
Key words: self-emulsifying styrene acrylate; decorative base paper; surface-treatment; printability; absorbability
Decorative paper，widely used in the surface
finishing of wood-based panel，can not only protect the
wood-based panel from wear，heat and contamination，
but also endow the products with excellent visual
effects( Paula，2012; Tan，2006) ． The properties of
decorative paper are determined by the properties of
the decorative base paper directly． Among the
performance indices of decorative base paper，the two
key indices are printability and absorbability． The
former affects the print quality and the latter affects the
absorption of melamine in the production of decorative
paper (Santos et al．，2005; Liu et al．，2007) ． Hence，
a huge demand for decorative base paper with good
absorbability and printability exists．
Surface treatment is considered as an effective
method to meet the demand，because it is crucial in
obtaining good printability，surface property，shape
stability and excellent physical strength of paper．
However， good water-resistant and oil-resistant
ability of paper is got by traditional manufacturing
method，which adversely affects the absorbability of
decorative paper ( Hu et al．， 2008; Xu et al．，
2012 ) ． In the present study， a series of self-
emulsifying SAE were synthesized by introducing
acrylic acid as the functional monomer． The carboxyl
of acrylic acid not only provides the hydrophilicity for
latex but also reacts with other monomers． The
crosslinking reaction between acrylic acid and other
monomers endows the product with good film forming
property， which leads to excellent printability of
paper sheets ( Zhang et al．，2011; Wang et al．，
2006 ) ． Subsequently， the effect of dosages of
acrylic and initiator and the mass ratio of hard
monomer ( styrene ) withsoft monomer ( butyl
acrylate) on the performance of SAE and its surface-
treatment behavior were determined． Finally， the
emulsion properties of self-emulsifying styrene
acrylate and the paper properties were determined．
1 Experimental
1. 1 Materials
The styrene (St)，acrylic acid (AA)，butyl acrylate
( BA )， methyl methacrylate ( MMA )， ammonium
persulfate (APS) and sodium bicarbonate used were all
analytically pure． The starch used in surface treatment
was cassava starch and the α-amylase was BＲ．
Decorative base paper with base weight of 110 g·m － 2 was
supplied by Shandong Zhengda Paper Co．，Ltd． SAE was
synthesized in laboratory．
1. 2 Preparation of self-emulsifying SAE
Firstly，an amount of distilled water was poured
into a four-port flask with a stirring device， a
condensing device and a thermometer． After adding a
certain quantity of sodium bicarbonate to the reactor，
1 /3 mixed monomers ( St，MMA，AA and BA，MMA
was used as a type of hard monomer with the dosage of
2wt% ) and 1 /3 initiator (APS，10wt% ) were added
to the flask while stirring，keeping the temperature
80 ℃ ． When the blue light appeared， the residual
monomers were added dropwise within 60 min，
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林 业 科 学 51 卷
whereas the residual initiator was added within 90 min．
The temperature was then raised to 85 ℃ and
maintained for 1. 5 h． Finally， the self-emulsifying
SAE latex was obtained and purified，by standing，
separating by separating funnel and filtering， for
further evaluation．
The reaction of AA was as follows
師
師帪
:
CH—CH

·
+ COOH
CH = CH

2
+ Ｒ →
師
師帪
2

CH CH 2CH

COOH
CH2—Ｒ 2
1. 3 Characterization
A microscopic infrared spectroscopy ( Nicolet
iN10) was utilized to characterize the chemical groups
on the paper． The emulsion particle morphology and
the surface morphology of paper were both observed
under a scanning electron microscopy ( SEM) system
( JEOL JSM-5310 ) and a laser particle sizer
(Brookhaven 90Plus) was used to measure the particle
size at a concentration of 0. 01% ． The charge density
of latex was measured by a particle charge detection
(PCD) system ( BTG，PCD03) at a concentration of
10 － 4 g·L － 1 ． The viscosity was measured by a rotational
viscometer (Chuang Yu，NDJ-79) at the rate range of
1 － 100 r·min － 1 ． The emulsion stabilities，including
mechanical，storage， pH， calcium ion and dilution
stability， were also investigated ( Warson et al．，
2001) ．
1. 4 Surface treatment of self-emulsifying SAE
A certain amount of starch was cooked with the
addition of α-amylase and the concentration was
regulated to 10% by adding water． The gelatinized
starch and self-emulsifying SAE were mixed with the
weight ratio 20 ∶ 1． Surface treatment was performed at
a concentration of 10% from 60 ℃ to 70 ℃ and the
coating weight was 7 － 8 g·m － 2 ． Based on a previous
study (Xu et al．，2013)，the films were prepared by a
drawdown using wire-wound bars and dried on a glazer
at 105 ℃，kept for 5 min．
1. 5 Physical properties of the paper sheets
The surface strength and absorbability ( capillary
rise ) of the treated paper sheets were measured
according to ISO 3783—2006 and ISO 8787: 1989，
respectively．
2 Ｒesults and discussion
The single factor experiment was designed and the
influencing factors，such as the dosage of acrylic acid，
the dosage of initiator，the mass ratio of hard monomer
with soft monomer，were studied．
2. 1 Effects of the AA dosage on the particle size，
charge density and surface-treatment behavior
of SAE
2. 1. 1 Effect of the AA dosage on the particle size
and charge density of SAE In the preparation of
SAE，acrylic acid was introduced as the functional
monomer． The carboxyl of acrylic acid not only
provides the hydrophilicity for latex but also reacts with
other monomers． The crosslinking reaction between
acrylic acid and other monomers endows the product
with good film forming property， which leads to
excellent printability of paper sheets．
The particle size affects the emulsion performance
and its application． In general， small and narrowly
distributed particle size contributes to excellent
emulsion performance． In addition，moderate charge
density of latex leads to stronger interaction between
emulsion and electronegative paper fiber． Thus，these
two indices are of particular interest．
When the APS dosage was 0. 3%，the ratio of St
with BA was 1. 5 ∶ 1 and the dosage of MMA was
2wt%，the effect of the AA dosage on the performance
of SAE was investigated and the result was shown in
Fig． 1．
Fig． 1 Effect of the AA dosage on the particle
size and charge density of SAE
Fig． 1 showed that with the increased AA dosage，
the emulsion particle size decreased at first then
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第 3 期 徐建峰等: 装饰原纸用自乳化苯乙烯丙烯酸酯表面处理剂的制备及表征
increased and the charge density increased． The
finding was due to the increased carboxyl with
increased dosage of AA，which led to an increased
anionic degree of emulsion． The hydrophilic groups
also increased and the polymer chains easily dispersed
(Xu et al．，2013; Chen et al．，2002; Dziomkina et al．，
2006)，so the SAE particle size decreased． When the
dosage of AA was larger than 8%，with increased
charge density of polymer molecular chains， the
electrostatic repulsion of emulsion particles increased，
which led to decreased interaction between the particles
(Wu et al．，2009) ． As a result，the emulsion particle
size became larger．
2. 1. 2 Effect of the AA dosage on the surface-
treatment behavior of SAE The surface strength of
paper sheet was selected to represent the printability in
terms of the pick velocity and pick resistance of paper
and in terms of the delamination resistance of the liner
on paper，by simulating the behavior in the printing
process． The capillary rise was selected to indicate the
absorbability of paper sheet． Thus，the surface strength
and capillary rise of decorative base paper are of
particular interest．
Under the same reaction conditions as Fig． 1，the
effect of the AA dosage on the surface-treatment
behavior of SAE was investigated and the result was
shown in Fig． 2．
Fig． 2 Effect of the AA dosage on the surface-
treatment behavior of SAE
As shown in Fig． 2，increased AA dosage led to
increased capillary rise of paper sheet． This finding
can be attributed to the increased AA dosage causing
the amount of hydrophilic carboxyl to increase on the
emulsion molecular chains． As a result， the
absorbability of paper sheet， treated by SAE，
increased．
Fig． 2 also showed that with the increase of AA
dosage，the surface strength of paper sheet initially
increased and then decreased． It was because that
the crosslinking reaction between AA with carboxyl
and other monomers could endow the product with
good film forming property． Within the certain range
(5wt% － 9wt% )，the dosage of AA was larger，the
film forming property was better and the surface
strength of paper sheet increased． However，when
the AA dosage was larger than 8% ，the particle size
increased ( shown in Fig． 1 ) ． Owing to the big
particle size，the polymer film on paper surface was
not compact and poor film was got， the surface
strength of paper sheet decreased．
Finally，the optimum AA dosage of 8wt% was
obtained with smaller particle sizes and moderate
charge density，which led to higher absorbability and
higher surface strength of paper sheet．
2. 2 Effect of the APS dosage on the particle size，
charge density and surface-treatment behavior
of SAE
2. 2. 1 Effect of the APS dosage on the particle
size and charge density of SAE The dosage of
initiator has critical effect on the performance of latex．
In this study，APS was chosen as the initiator and its
dosage was investigated．
When the AA dosage was 8wt%，the ratio of St
with BA was 1. 5 ∶ 1 and the dosage of MMA was
2wt%， the effect of the APS dosage on the
performance of SAE was investigated and the result was
shown in Fig． 3．
Fig． 3 Effect of the APS dosage on the particle
size and charge density of SAE
From Fig． 3，it was shown that with the increase
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林 业 科 学 51 卷
of the APS dosage，the particle size decreased at first
then increased and the opposite trend of charge density
of emulsion was observed．
With the increase of the APS dosage， the
formation rate of free radicals and the chain termination
rate increased， leading to lower average molecular
weight of polymer，and small particle size was got．
When the APS dosage was larger than 0. 4%，with the
increased APS dosage， the termination rate of
polymerization increased and the reaction rate relatively
decreased． Thus the amount of latex particles，which
participated in the reaction， became small and the
particle size of latex became bigger．
On the other hand，when the dosage of APS was
small， the reaction rate was low， resulting in the
residual of some of the monomers． Because of the
presence of residual monomers，the conversion of AA
with carboxyl，was low，leading to low charge density
of emulsion． And with the increase of APS dosage，the
amount of the free radicals became larger and the rate
of polymerization became faster， leading to high
conversion of AA． Because of more anionic groups
provided by AA on the polymer molecular chain，
higher charge density of emulsion was obtained． When
the APS dosage of was larger than 0. 4%， the
conversion of AA increased little and the charge density
of latex almost unchanged．
2. 2. 2 Effect of the APS dosage on the surface-
treatment behavior of SAE Under the same
reaction conditions as Fig． 3， the effect of the APS
dosage on the surface-treatment behavior of SAE，
including the surface strength and capillary rise，of
decorative base paper were investigated． as shown in
Fig． 4．
It was shown in Fig． 4 that the surface strength of
paper sheet，treated by SAE，increased at first then
decreased and the opposite trend of capillary rise was
observed． It was because with the increase of the APS
dosage ( from 0. 1% to 0. 4% )，the particle size of
latex decreased ( shown in Fig． 3) ． So the permeation
and film formation of polymer on the paper surface was
easy， which was helpful for the formation of good
polymer film． As a result，the surface strength of paper
sheet increased． When the APS dosage was larger than
0. 4%，the particle size of SAE became bigger and it
was not close for the stacking of the particles when the
polymer film formed，leading to the formation of poor
film． So the surface strength of paper sheet decreased．
In addition，with the increase of the APS dosage，
the particle size of SAE decreased at first then
increased ( shown in Fig． 3) ． When the particle size
was small，it was close for the stacking of the particles
when the polymer film formed，so it was difficult for
the water’s permeation into the film， which was
presented as low capillary rise． Oppositely，when the
particle size became larger，poor film on the paper
surface was got and it was easy for the permeation of
water into film． So the capillary rise increased．
Finally，the optimum APS dosage of 0. 4% was
obtained with smaller particle sizes and moderate
charge density，which led to higher absorbability and
higher surface strength of paper sheet．
Fig． 4 Effect of the APS dosage on the
surface-treatment behavior of SAE
2. 3 Effect of the mass ratio of St with BA on the
particle size，charge density and surface-treatment
behavior of SAE
2. 3. 1 Effect of the mass ratio of St with BA on
theparticle size and charge density of SAE
Different monomers have different film-forming property
and hydrophobic property． So the dosage of each
monomer is crucial for the performance of SAE． When
the AA dosage was 8wt%，APS dosage was 0. 4% and
the dosage of MMA was 2wt%，the effect of St with BA
on the performance of SAE was investigated and the
result was shown in Fig． 5．
From Fig． 5，we could see that the particle size of
emulsion changed little with the change of the mass
ratio of St with BA， whereas the charge density
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第 3 期 徐建峰等: 装饰原纸用自乳化苯乙烯丙烯酸酯表面处理剂的制备及表征
decreased． The finding was due to the higher reactivity
of St than other monomers ( including BA)，which led
to the self-polymerization of St， rather than the
copolymerization of AA and St． When the mass ratio of
St with BA increased，the anionic groups provided by
AA on the polymer molecular chain decreased and the
smaller charge density of emulsion was obtained． And
the ratio of St with BA had little effect on the emulsion
particle size．
2. 3. 2 Effect of the mass ratio of St with BA on
the surface-treatment behavior of SAE Under the
same reaction conditions as Fig． 5，the effect of the St
with BA on the surface-treatment behavior of SAE，
including the surface strength and capillary rise，of
decorative base paper were investigated，as shown in
Fig． 6．
It was shown in Fig． 6 that with the increase of the
mass ratio of St with BA，the surface strength of paper
sheet， treated by SAE， increased at first then
decreased and the capillary rise increased．
The more the hard monomer ( St ) was，which
endowed the polymer film high strength and hardness，
the better film was got． So the surface strength of paper
sheet increased． When the mass ratio of St with BA
was larger than 1. 5 ∶ 1，the hardness of polymer film
became too high and the film became brittle，shown as
decreased surface strength．
On the other hand，the film-formation property of
BA was better than St，so when the mass ratio of St
with BA increased，looser film was obtained and the
capillary rise of paper sheet decreased．
Finally，the optimum mass ratio of St with BA of
1. 5 ∶ 1 was obtained with smaller particle sizes and
moderate charge density， which led to higher
absorbability and higher surface strength of paper
sheet．
2. 4 Characterization
2. 4. 1 Characterization of emulsion The
performance of self-emulsifying SAE prepared under
the optimum conditions，such as 8wt% AA，0. 3wt%
ammonium persulfate，mass ratio of styrene ( St) to
butyl acrylate ( BA ) 1. 5 ∶ 1，was studied and the
results were shown in Tab． 1． Excellent emulsion
performance was obtained in the laboratory， i． e．，
small particle sizes， low viscosity，moderate charge
Fig． 5 Effect of the mass ratio of St with BA on the
particle size and charge density of SAE
Fig． 6 Effect of the mass ratio of St with BA on the
surface-treatment behavior of SAE
density and good stability． Fig． 7 showed that the SAE
particles were spherical and with core- shell structure，
which endowed the emulsion low film forming
temperature，good stability and excellent mechanical
properties ( Zhang et al．，2008 ) ． From Fig． 8，we
observed that the particles were well distributed，with
the average diameter around 130 nm．
2. 4. 2 Characterization of paper sheets A
microscopic infrared spectroscopy was utilized to
characterize the chemical groups on the paper and the
surface morphology of paper sheets were observed
under a scanning electron microscopy． Fig． 9 showed
that compared to untreated paper and the paper treated
by starch，the peak at 1 727 cm － 1 was observed on the
paper sheet treated by SAE，which indicated there was
carbonyl of carboxylic． From Fig． 10，we could see
that compared to the other paper sheets，more surface
of paper，treated by SAE，was covered by film． For
the paper sheet， treated by SAE， carboxyl on the
paper endowed good absorbability and the polymer film
endowed excellent printability．
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林 业 科 学 51 卷
Tab． 1 Performance of SAE prepared in lab
Property
Solids content(% ) 35
Particle size / nm 130
Charge density /(mmol·L － 1 ) 0. 70
Viscosity /(mPa·s) 20
Mechanical stability Stable
Storage stability stability Stable during 90 days
pH stability 9 － 1
Calcium ion stability Stable，has no layered
Dilution stability Stable
Fig． 7 Particle morphology of SAE
Fig． 8 Particle size distribution of copolymer latex
Fig． 9 Microscopic infrared spectroscopy of paper sheets
And the surface-treatment effect of SAE was
shown in Tab． 2． From the table，we could see that for
the paper treated by SAE，the capillary rise had little
change and the surface strength and smoothness had
been improved greatly，compared with the values of
untreated paper and national standard． The paper
treated by starch had poor absorbability ( shown as low
capillary rise) and surface strength．
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第 3 期 徐建峰等: 装饰原纸用自乳化苯乙烯丙烯酸酯表面处理剂的制备及表征
Fig． 10 SEM of paper sheets
Tab． 2 Physical properties of decorative base paper after surface treating①
Capillary rise /［mm·(10 min) － 1］ Surface strength /(m·s － 1 ) Smoothness / s
Untreated paper 20 0. 8 105
Paper treated by self-made SAE 19 1. 1 130
Treated by starch 16 0. 9 110
National standard 20 — 100
①The national standard is GB /T 24989—2010．
3 Conclusions
Self-emulsifying latex with excellent performance
was obtained under the following conditions: 8wt%
AA， 0. 3wt% ammonium persulfate， mass ratio of
styrene (St) with butyl acrylate (BA) 1. 5∶ 1，130 nm
emulsion particle size，moderate charge density of the
emulsion and low viscosity． An excellent surface-
treatment effect was obtained under these conditions．
The surface-treated paper was covered by film
partially and carboxyl was observed on the paper． The
printability of decorative base paper，treated by self-
emulsifying SAE， significantly improved and the
absorbability of paper sheet was maintained．
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