Received: 4 March 2020 Revised: 11 June 2020 Accepted: 14 June 2020

DOI: 10.1002/app.49683

ARTICLE

Modification of the wood-plastic composite for

enhancement of formaldehyde clearance and the 3D
printing application

Qi Jiang1 | Yifan Xu1 | Mingliang Chen2 | Qinghua Meng1 | Chongyin Zhang3

1
School of Chemistry and Chemical
Engineering, Shanghai Jiao Tong
Abstract
University, Shanghai, China As the formaldehyde is one of the main indoor pollutants, the purpose of this
2
Shanghai Aerospace System Engineering study is to effectively remove indoor formaldehyde pollution by using environ-
Institute, Shanghai, China
mentally friendly 3D printing ornaments. The wood 3D printing filaments cel-
3
Shanghai Engineering Research Center
of Specialized Polymer Materials for
lulose/polylactic acid composite (Cellu/P) was selected as the starting material,
Aerospace, Shanghai Aerospace and 3-aminopropyltriethoxysilane (APTES) was used for chemical modifica-
Equipments Manufacturer Co., Ltd, tion to obtain a series of cellulose composite materials with amino groups. The
Shanghai, China
modified composite materials (APTES@Cellu/P) were characterized by Fou-
Correspondence rier transform infrared, X-ray diffraction, scanning electron microscope,
Qinghua Meng, School of Chemistry and energy dispersive spectroscopy, thermogravimetric analysis, and mechanical
Chemical Engineering, Shanghai Jiao
Tong University, Shanghai 200240, China. tests, and a formaldehyde removal experiment was performed. The feasibility
Email: qhmeng@sjtu.edu.cn of 3D printing was evaluated, and the process of 3D printing-functionalized
customized ornaments was proposed, and then a school emblem was used for
Chongyin Zhang, Shanghai Engineering
Research Center of Specialized Polymer modeling, printing, and surface modification. Compared with the commer-
Materials for Aerospace, Shanghai cially traditional activated carbon, 3D printing-customized ornaments of
Aerospace Equipments Manufacturer Co.,
Ltd. Shanghai 200245, China.
APTES@Cellu/P material has a better formaldehyde removal effect, and can
Email: chongyin1022@163.com even avoid the secondary pollution that is common to the activated carbon.

KEYWORDS
biodegradable, biopolymers and renewable polymers, cellulose and other wood products

1 | INTRODUCTION At present, the common methods to remove formal-

Formaldehyde (HCHO) is a harmful, pathogenic indoor
air pollutant, which is one of the carcinogens and terato-
gens recognized by the World Health Organization.1,2 As
a representative indoor pollutant, formaldehyde mainly
comes from indoor furniture paints, decorative materials,
polymer boards, adhesives, and chemical fiber carpets.3
High levels of formaldehyde can cause a range of symp-
toms, including pharyngitis, rhinitis, emphysema, lung
cancer, and even death.4 Therefore, taking effective
removal of formaldehyde in indoor air become the focus
of our research.5
dehyde from indoor air are thermal catalytic oxidation
decomposition,6 green plant purification,7,8 photo-
catalytic degradation,9–11 plasma technology,12 and
adsorption method.13–15 Adsorption method is the most
common method today. Activated carbon is widely used
due to its large specific surface area, pore structure, rich
oxygen-containing functional groups on the surface, easy
access, and low price.16 However, the use of activated car-
bon has certain limitations. After adsorbing pollutants,
such as formaldehyde, its reversibility will lead to desorp-
tion probably when environmental factors including tem-
perature, humidity, or other factors change, and thus

J Appl Polym Sci. 2020;e49683. wileyonlinelibrary.com/journal/app © 2020 Wiley Periodicals LLC 1 of 10

https://doi.org/10.1002/app.49683
2 of 10
result in secondary pollution. It is necessary to further
develop new formaldehyde purification materials that
can replace activated carbon. Recently, as the formation
of Schiff bases from amino groups can effectively interact
with formaldehyde,17,18 surface amine modification has
become an effective method to improve the formaldehyde
adsorption performance and solve the problem of second-
ary pollution.
Natural fiber materials mainly refer to materials
containing cellulose, which is the most abundant form
of renewable natural resources.19 Cellulose is a polysac-
charide composed of cellobiose which is linked with
each other by β-1,4-glycosidic bond to form a long
molecular chain.20 The presence of plenty of hydroxyl
groups distribute on the surface of cellulose contributes
to the adsorption performance,3 and meanwhile pro-
vides the possibility of functional modification
reactions,21 such as esterification, etherification, graft
copolymerization, and oxidation. In recent years, the
natural fiber composite materials have also emerged
and benefit in terms of positive environmental impact,
such as recyclability, renewability, and biodegradabil-
ity.19 Among them, composite materials prepared by
blending natural plant fibers with biodegradable poly-
lactic acid (PLA) have become commonly used 3D
printing green materials. Thus, we intend to carry out
surface modification of natural plant fiber/PLA com-
posite 3D printing material for the purpose of a thor-
ough removal of formaldehyde.
In view of this, we use 3-aminopropyltriethoxysilane
(APTES) to surface modify the cellulose/polylactic acid
compound material (Cellu/P) for better removal of form-
aldehyde. The surface morphology and absorption perfor-
mance will be evaluated and the feasibility for 3D
printing will be discussed as well.
2 | EXPERIMENTAL
2.1 | Materials
All reagents used in the experiments are of analytical
grade and can be used without further purification.
Deionized water was used in all experiments.
APTES was purchased from Shanghai Chemical
Reagent (China). Concentrated sulfuric acid (98%)
and acetone were purchased from Sinopharm Group
Chemical Reagent (China). Wood composite filament
for 3D printing (Cellu/P) was purchased from
Aurora (China), in which the proportion of wood
powder and PLA is 85:15. Commercial activated car-
bon block was purchased from Juyile environmental
(China).
JIANG ET AL.
2.2 | Modification of materials
As the pretreatment of preparation of powder sample of
APTES@cellu/P for requirement of some measurements,
the Cellu/P filament was initially crushed to powder
(about 200 mesh) by a M150A universal high-speed
grinder (Tianxi, China).
Preparation of the filament and 3D printing ornament
samples of APTES@cellu/P directly used the cellu/P fila-
ment and 3D printing cellu/P ornament, respectively,
and went to the following activation and modification
processes according to Caicedo's method.22
Activation process: The flask was added with 10 g of
Cellu/P and 140 ml of 35 wt% sulfuric acid, and reacted
for 6 h at constant temperature of 60
C. The activated
cellulose composite (act_Cellu/P) was prepared by wash-
ing the surface of the material with deionized water to
remove the hydrogen ion and sulfate ion, filtering, and
drying at 60
C.
Modification process: The ethanol solution of APTES
(0.1–1 M) with different concentrations was used as the
modifier solution. The flask was added with 5 g of
act_Cellu/P and 100 ml of modifier solution. The pH
value was adjusted to 3–4 with hydrochloric acid during
stirring. The reaction was performed at room tempera-
ture for 15 min, and then heated to 60
C for 3 h. Filtered
by suction and washed with 100 ml acetone, the modified
cellulose composite (APTES@cellu/P) was prepared after
air drying at room temperature.
The percentage of modification ratio (MR) was calcu-
lated using Equation (1),
m2 − m1
FC = × 100%, ð1Þ
m1
where m1 was the weight of act_Cellu/P, and m2 was the
weight of APTES@Cellu/P.
2.3 | Characterization of materials
The Fourier transform infrared (FTIR) spectra were
recorded on a Nicolet iS5 FTIR spectrophotometer
(Thermo Fisher, USA) in a water-purged environment.
All spectra were obtained from compressed KBr pellets in
which the samples were evenly dispersed. Further,
32 scans were used to record each FTIR spectrum with a
2 cm−1 spectral resolution at room temperature.
The morphology and elemental analysis were ana-
lyzed at 15 kV accelerating voltage by a Nova NanoSEM
450 scanning electron microscope (SEM) (FEI, USA)
equipped with an energy dispersive spectroscopy (EDS)
analysis system. Under the condition of 80,000 times
JIANG ET AL. 3 of 10

magnification, the scanning of point element content and

the scanning of surface element content are measured.
The N2 adsorption isotherm was measured on an
ASAP 2010 M+C surface area and porosimetry analyzer
(Micromeritics, USA). Before nitrogen adsorption mea-
surement, degas all prepared samples at 180
C.
Brunauer-Emmett-Teller (BET) surface area was deter-
mined by multipoint BET method using adsorption data
with relative pressure (P/P0) in the range of 0.05–0.3.
The X-ray diffraction (XRD) analysis of the samples
were conducted on a D8 advance X-ray diffractometer
(Bruker, Germany).
The thermal stability of the sample was evaluated by
the thermogravimetric analysis (TGA) on a Discovery
TGA550 thermal analyzer (TA, USA) at a heating rate of
20
C/min in nitrogen atmosphere.
The mechanical property tests including elastic modu-
lus, tensile strength, and elongation at break were per- F I G U R E 1 The creation route of the modeling file for custom-
formed on an Instron 4465 Universal Testing Machine made 3D printing [Color figure can be viewed at
(Instron, USA). All the tests were based on filaments of wileyonlinelibrary.com]
30 mm in length and 7 mm in diameter, and conducted in
a temperature- and humidity-controlled room (20
C tem-
perature and 40% Relative Humidity). The cross-head speed detection chamber (Figure S1) with reference to the liter-
of 5 mm/min was adopted and the mean value for each ature methods.1,10,11,18 After the formaldehyde adsorbent
mechanical property was obtained from at least five tests. sample was placed at the temperature control platform,
the chamber was sealed. After starting the fan on the
bulkhead, 5.83 ml of 0.3% formaldehyde gas was injected
2.4 | 3D modeling and printing from the injection port with a syringe and the peak value
of the initial concentration c0 was recorded immediately.
Original 2D vector image according to customized The change value (ct) of the formaldehyde detector was
requirements was imported into Materialize's Interactive recorded over time, and the fan worked continuously
Medical Image Control System (MIMICS, Materialize, during the whole removal process. Turn off the fan and
Belgium). To separate the printing part, threshold was set stop the experiment until the formaldehyde detector
according to the gray level of the image. 3D model was reading decreased to the constant value. (To investigate
imported into Unigraphics NX (UG NX, Siemens, Ger- the thoroughness of formaldehyde removal, the sample
man). According to the size of the printing target, a model could be heated after its removal equilibrium.) The per-
was established to generate a 3D printing file (Figure 1), centage of formaldehyde clearance (FC) was calculated
which was to be imported into the 3D printer for printing. using Equation (2),
Fused Deposition Molding (FDM) type 3D printer
Finder (FlashForge, China) was used for printing. Print- c0 −ct
FC = × 100%: ð2Þ
ing was carried out layer by layer by copper nozzle (diam- c0
eter of 350 μm). The layer thickness was set to 0.08 mm,
the reference printing speed was set to 60 mm/s, and the
filling degree is set to 60%.
The modification of printed 3D printing ornament 3 | RESULTS A ND DISCUSSION
was according to the procedure in Section 2.2 Modifica-
tion of materials. 3.1 | Modification of materials

3.1.1 | Modification reaction

2.5 | Formaldehyde removal experiment
For better efficiency of formaldehyde removal, Cellu/P
Formaldehyde removal experiment was carried out at has been chemically modified using APTES. The mecha-
temperature of 25
C in a self-made plexiglass air nism (Figure 2) is that the hydroxyl groups on cellulose
4 of 10 JIANG ET AL.

Cellu/P
OH
O OH
O HO
HO O
Transmittance (a.u.) OH O

OH n

APTES@Cellu/P H+ APTES

NH2
-NH2
-NH2 C2H5O
C2H5O Si

C-O-Si O

O OH
O HO
3500 3000 2500 2000 1500 1000 HO O
-1 OH O
Wavenumber (cm )
OH n

F I G U R E 2 Modification of Cellu/P composite by APTES and their FTIR spectra of the powder samples. APTES,
3-aminopropyltriethoxysilane; FTIR, Fourier transform infrared [Color figure can be viewed at wileyonlinelibrary.com]

(a) (b)
3.0
3.0

2.5
2.5
Modification ratio(%)

Modification ratio(%)

2.0
2.0

1.5 1.5

1.0 1.0

0.5 0.5

0.0 0.0

0.0 0.1 0.2 0.3 0.4 0.5 0 1 2 3 4 5

APTES concentration (M) Time (hr)

F I G U R E 3 The effects of the APTES concentration (a) and reaction time (b) on the modification ratio of Cellu/P of the filament
samples. APTES, 3-aminopropyltriethoxysilane

are activated by acid, which attacks the silylethoxyl group that amino group was successfully introduced into the
on APTES, and then eliminates a molecule of ethanol to molecular structure of cellulose composite after APTES
form C O Si ether bond, so as to obtain the modified modification, which may function in air purification.
cellulose composite APTES@cellu/P. The new absorption In view of the modification reaction of cellu/P mate-
band near 1150 cm−1 in FTIR spectrum can be attributed rial, the effects of concentration of solution and reaction
to the asymmetric stretching vibration of C O Si time on the MR of APTES were studied. As shown in
bond.23 Furthermore, compared with cellu/P material, Figure 3(a), with the increase concentration of APTES,
the absorption band of APTES@Cellu/P modified mate- the MR increased continuously, reaching the equilibrium
rial near 3480 cm−1 can be attributed to the stretching value when APTES concentration reaches 0.3 M, and the
vibration of primary amine N H bond,24 and its broad MR almost remained unchanged with the further
band covers the characteristic band of hydroxyl group in increase of APTES concentration. As shown in Figure 3
this region. The new absorption band near 1466 cm−1 (b), with the increase of APTES reaction time, the MR
can be attributed to the symmetric bending vibration of was also increasing, and the equilibrium ratio was
primary amine N H18 (Figure 2). It can be confirmed reached after the modification reaction time reached 3 h.
JIANG ET AL.
XRD was used to study the crystal structure of
APTES@Cellu/P. As shown in Figure 4, compared with
cellu/P material, the main peak of APTES@Cellu/P mod-
ified material is shifted from 17
to 22
and the position
of the peak can be attributed to the 200 crystal plane dif-
fraction of cellulose, which confirmed the modification of
APTES on cellu/P to some extent.25
3.1.2 | Surface morphology
Activation and modification of cellu/P composite fila-
ment (Figure 5(a)) would inevitably change the physical
and chemical condition of the surface. SEM and EDS
were used to study the surface of the filament. As can be
seen from Figure 5(b), the surface of cellu/P composite
was basically smooth and flat, with only tiny processing
stripes and a few pores (diameter <5 μm).
After acid activation, there were some cracks on the
surface of the sample (act_Cellu/P) due to the swelling of
hydrophilic cellulose and along the direction of the origi-
nal processing stripe of the filament. The gap width was
about 10 μm (Figure 5(c)), and EDS data showed that the
content of oxygen element on the surface of the material
increased (Figure 5(e)), indicating that the concentration
of free hydroxyl group on the surface of the material
increased after activation, which was conducive to the
subsequent modification reaction.
After the modification reaction of APTES (APTES@
Cellu/P), the defects on the surface of the material fur-
ther developed and the cracks also expanded, and the
Cellu/P
Intensity (a.u.)
APTES@Cellu/P
10 20 30 40 50 60 70
2θ ( )o
F I G U R E 4 The XRD spectra of Cellu/P and APTES@Cellu/P
of the powder samples. APTES, 3-aminopropyltriethoxysilane;
XRD, X-ray diffraction [Color figure can be viewed at
wileyonlinelibrary.com]
5 of 10
maximum gap width could exceed 50 μm (Figure 5(d)).
The EDS data showed that the content of silicon element
on the surface of the material increased significantly
(Figure 5(e)), which indicated the chemical bonding of
APTES on the surface of the material. In addition, through
the elements scanning of EDS (Figure S2), it was found
that the enrichment of silicon on the surface defects,
where also indicated the reaction of APTES proceeded
preferentially (Figure 5(f), (g)).
These surface defects would reduce the mechanical
properties of the material. On the other hand, defects
would lead to a large specific surface area. It can be seen
from the nitrogen adsorption measurement (Figure S3)
that the specific surface area increased from the value of
1.24 m2/g (Cellu/P) before modification to the value of
2.73 m2/g (APTES@Cellu/P) after modification, which
showed the modified material had better purification
function than the unmodified material.
3.2 | Purification of the formaldehyde
The aldehyde group in formaldehyde molecule can be
adsorbed by formation of hydrogen bond with cellulose
hydroxyl group. However, hydrogen bond is a weak and
reversible interaction, which can release the formalde-
hyde under certain conditions. Therefore, the purification
capacity of unmodified cellulose material is weak and
lack the value of practical use.26 In this work, the modi-
fied cellulosic material (APTES@Cellu/P) with amino
groups can form Schiff base through condensation reac-
tion to achieve the purpose of efficient formaldehyde
removal (Figure 6). The absorption band of material at
1466 cm−1 on FTIR curve of APTES@Cellu/P ascribed to
the symmetrical bending vibration of primary amine
( NH2). After reaction with formaldehyde, the band of
primary amine ( NH2) was obviously weakened, while
the new band at 1645 cm−1 appeared that belonged to the
stretching vibration of C N bond of Schiff base
(Figure 6).27
In view of this, APTES@Cellu/P materials were fur-
ther studied. According to the samples of
APTES@Cellu/P with different modified ratios, the
removal efficiency of formaldehyde gas was investigated
in the air detection chamber (Figure S1). As shown in
Figure 7(a), each sample had a rapid formaldehyde
removal stage in the initial stage. As the formaldehyde
removal rate increased gradually, the removal rate
decreased gradually until the final balance, and the
adsorption kinetics had a good fitness to the pseudo sec-
ond order kinetic (Figure S5). In addition, the final values
of FC was found linear with APTES MR roughly
(Figure 7(b)). The APTES@Cellu/P material with a MR
6 of 10 JIANG ET AL.

F I G U R E 5 The surface morphology of Cellu/P, act_Cellu/P, and APTES@Cellu/P of the filament samples. (a) The diagram of
modification on the microscopic interface. (b) The SEM image of Cellu/P. (c) The SEM image of Act_Cellu/P. (d) The SEM image of
APTES@Cellu/P. (e) The EDS analysis of Cellu/P, Act_Cellu/P, and APTES@Cellu/P. (f) and (g) The EDS scanning on a defect area of
APTES@Cellu/P by Si mode. APTES, 3-aminopropyltriethoxysilane; EDS, energy dispersive spectroscopy; PLA, polylactic acid; SEM,
scanning electron microscope [Color figure can be viewed at wileyonlinelibrary.com]

of 2.68% showed a maximum final FC of 77% and the
adsorption capacity was estimated as 10.98 μg/g
(Figure S6).
3.3 | 3D printing application
3.3.1 | Assessment of the printability
As the filament needs to go through a heating nozzle of
nearly 300
C in FDM 3D printer, TGA was used to evalu-
ate the thermal stability of APTES@Cellu/P material,
and unmodified Cellu/P material was used as a reference.
As seen from TGA (Figure 8(a)), the thermal decomposi-
tion of APTES@Cellu/P material was mainly divided into
three stages. The first thermal degradation stage of
70 ~ 120
C was ascribed to the decomposition of ethoxyl
groups on APTES@Cellu/P and the Si O bond was then
formed (Figure S4). The second thermal degradation
stage of 300 ~ 360
C was ascribed to the decomposition
and carbonization of cellulose and PLA. In this process,
the weight loss of organic matter was faster and more.
The weight loss inflection point of APTES@Cellu/P
appeared at about 310
C, which was about 15
C higher
than that of unmodified Cellu/P, indicating that the mod-
ification of cellulose by organosilicon improved the ther-
mal stability of the material to some certain extent. The
third thermal degradation stage of 360 ~ 500
C was
ascribed to the decomposition of propylamino group from
silicon and further carbonization of the material to form
carbon silicon hybrid material.28
3D printing filament materials for the FDM type
printer generally undergo screw extrusion and stretch,
which have high requirements on the mechanical
JIANG ET AL. 7 of 10

NH2

C2H5O
C2H5O Si

O
APTES@Cellu/P O HO
OH
O
HO O O
OH
Transmittance (a.u.)

OH n

N-H H
O
H

HCHO+APTES@Cellu/P H
N

C2H5O H
C=N C2H5O Si
O

O OH
O HO
2000 1800 1600 1400 1200 1000 800 HO O O
OH
-1
Wavenumber (cm ) OH n

F I G U R E 6 The reaction mechanism of the APTES@Cellu/P with the formaldehyde and the FTIR spectra of the powder samples.
APTES, 3-aminopropyltriethoxysilane; FTIR, Fourier transform infrared; HCHO, formaldehyde [Color figure can be viewed at
wileyonlinelibrary.com]

(a) (b) 100

100

80
80
2.68% APTES@Cellu/P
HCHO Clearance (%)

HCHO Clearance (%)

60 60
1.84% APTES@Cellu/P

1.28% APTES@Cellu/P 40
40

20 Cellu/P 20

0 0
0 5 10 15 20 25 30 0.0 0.5 1.0 1.5 2.0 2.5 3.0
Time (min) Modification ratio (%)

F I G U R E 7 (a) The variation of clearance of the APTES@Cellu/P filament samples along with the time at the initial formaldehyde
concentration of 3 mg/m3. (b) The effects of the modification ratio of APTES@Cellu/P filament samples on the final formaldehyde
clearance. APTES, 3-aminopropyltriethoxysilane; HCHO, formaldehyde [Color figure can be viewed at wileyonlinelibrary.com]

properties of filament materials as well. The Instron 4465 which may be caused by the porosity morphology after
material testing machine was used to study mechanical APTES's modification. Therefore, it was difficult for the
properties of APTES@Cellu/P, including elastic modulus, APTES@Cellu/P modified material to experience the
tensile strength, and elongation at break, and the process of direct extrusion preparation and printing
unmodified Cellu/P was used as the reference. The test directly using filament forms in terms of poor mechani-
results (Figure 8(b)) showed that the mechanical parame- cal properties. Instead, it was found suitable for the
ters of the modified APTES@Cellu/P material were sig- method of printing the unmodified Cellu/P filament
nificantly lower than those of the unmodified material, into an ornament and following functional modification
especially the tensile strength and elongation at break, on its surface.
8 of 10 JIANG ET AL.

(a) (b)
Cellu/P 270 Elastic modulus 60 60
100 APTES@Cellu/P Tensile strength at break
Elongation at break

Elongation at break (%)

Tensile strength (MPa)
Elastic modulus (MPa)
80 240 50 50
Weight (%)

100
60
95
210 40 40

40
90

180 30 30
20 85
260 280 300 320 340

0 150 20 20
100 200 300 400 500 600 Cellu/P APTES@Cellu/P
Temperature (°)

F I G U R E 8 (a) TGA and (b) The diagram of mechanical properties (elastic modulus, tensile strength, and elongation at break) of
Cellu/P and APTES@Cellu/P filament samples. APTES, 3-aminopropyltriethoxysilane; TGA, thermogravimetric analysis [Color figure can
be viewed at wileyonlinelibrary.com]

(a)

(b) (c) 3.0

80

70
HCHO concentration (mg/m )
3

2.5
Heating on Heating off
60
HCHO Clearance (%)

50 2.0

40
1.5
30
Active carbon
20
1.0
10 APTES@Cellu/P

0 0.5
Cellu/P APTES@Cellu/P Active carbon 0 20 40 60 80 100
Time (min)

F I G U R E 9 The 3D printing functional custom-made ornament and its behavior of formaldehyde clearance. (a) The route of 3D
printing custom-made ornament and the functionalization. (b) The comparison of formaldehyde clearance among ornaments of Cellu/P,
APTES@Cellu/P and commercial active carbon. (c) The effect of the following heating on the formaldehyde clearance. APTES,
3-aminopropyltriethoxysilane; HCHO, formaldeyde [Color figure can be viewed at wileyonlinelibrary.com]
JIANG ET AL.
3.3.2 | 3D printing of the functional
customized ornament and the practical
application on the formaldehyde removal
According to the actual application demands of users, the
process of 3D printing functional customized ornament
was established (Figure 9(a)). The emblem of Shanghai
Jiao Tong University was taken as a personalized exam-
ple, and its vector image can be the imported MIMICS
and UG NX software for processing. The data file for 3D
printing was obtained and then imported into FDM type
3D printer (FlashForge). The ornament was printed using
Cellu/P filament and the surface was modified with
0.3 M APTES solution to offer functional customized
ornament.
To evaluate its practical effect, 1 g sample was taken
from the ornament and the FC was measured in an air
detection chamber at room temperature (25
C), in which
the Cellu/P filament and a commercial active carbon
(Juyile) were parallelly measured, respectively, for com-
parison. It can be found that the 3D functional ornament
prepared by the modified material has the best formalde-
hyde removal effect (Figure 9(b)), which may have a good
application prospect. In order to investigate the thor-
oughness of formaldehyde removal, the sample was fur-
ther heated to 120
C (for 17 min) after reaching
equilibrium. Through parallel comparison (Figure 9(c)),
it was found that some formaldehyde was released from
the commercial activated carbon immediately (the form-
aldehyde concentration in the air detection chamber sud-
denly increased by 0.25 mg/m3), while the printed
sample of APTES@Cellu/P only resulted in very small
change of formaldehyde concentration (<0.03 mg/m3).
The comparative experiment showed that reversible
physical adsorption is the biggest problem of activated
carbon, which has monopolized the indoor air purifica-
tion market for a long history. Characteristically,
APTES@Cellu/P material can mainly lock and eliminate
formaldehyde thoroughly and the formaldehyde will not
relapse in case of temperature change.
4 | C ON C L U S I ON S
For better efficiency of formaldehyde removal, the modi-
fied natural fiber composite (APTES@Cellu/P) was pre-
pared through acid activation chemical reaction. The
effects of solution concentration and reaction time of
APTES on the modification rate was studied. The main
shift of XRD diffraction peak of the modified material
was observed, and the surface defects caused by the mod-
ification were found by SEM. The extent of APTES modi-
fication has a linear and decisive effect on the final
9 of 10
formaldehyde removal rate. APTES@Cellu/P material at
the modification rate of 2.68% showed the largest final
formaldehyde removal rate of 77%. The feasibility of 3D
printing of modified materials was evaluated, and the
process of 3D printing functional customized ornament
was established. In contrast to the commonly used active
carbon, APTES@Cellu/P material indicated its advan-
tages of higher FC and the irreversibity as well.
ORCID
Qinghua Meng https://orcid.org/0000-0002-5522-9852
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S UP PO RT ING IN FOR MAT ION
Additional supporting information may be found online
in the Supporting Information section at the end of this
article.
How to cite this article: Jiang Q, Xu Y, Chen M,
Meng Q, Zhang C. Modification of the wood-plastic
composite for enhancement of formaldehyde
clearance and the 3D printing application. J Appl
Polym Sci. 2020;e49683. https://doi.org/10.1002/
app.49683