Green Chemical Engineering xxx (xxxx) xxx

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Green Chemical Engineering

journal homepage: www.keaipublishing.com/en/journals/green-chemical-engineering

Shape-tailorable amine grafted silica aerogel microsphere for CO2 capture

Xing Jiang a, c, Jian Ren a, Yong Kong a, c, e, *, Zhiyang Zhao a, c, Xiaodong Shen a, c, e,
Maohong Fan b, d, **
a
College of Materials Science and Engineering, Nanjing Tech University, Nanjing, 210009, PR China
b
Department of Chemical and Petroleum Engineering, University of Wyoming, Laramie, WY, 82071, USA
c
Jiangsu Collaborative Innovation Center for Advanced Inorganic Function Composites, Nanjing, 210009, PR China
d
School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA
e
Suqian Advanced Materials Industry Technology Innovation Center of Nanjing Tech University, Suqian, 223800, PR China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

 A new amine grafted silica aerogel

microsphere (AGSAM) was developed.
 AGSAM was prepared with low-cost and
environmental-friendly raw material and
method.
 AGSAM had a CO2 adsorption capacity
of 1.04 mmol/g.
 The AGSAM with 4, 3.2, 2 and 1 mm in
diameters had the fluidizing velocities of
0.531, 0.425, 0.265 and 0.159 m -1,
respectively.
 AGSAM can be available on both fixed
bed and fluidized bed.

A R T I C L E I N F O A B S T R A C T

Keywords: The purpose of this study was to prepare a proof-of-concept CO2 adsorbing material based on a new amine grafted
Silica aerogel silica aerogel microsphere (AGSAM) that could be used on both fixed and fluidized beds. A low-cost water glass
Microsphere and environment-friendly water were used as precursor and solvent of the silica aerogel, respectively. The silica
Amine grafting
aerogel microsphere (SAM) was prepared by dropping the siliceous solution into hot oil bath. The effect of the pH
CO2 adsorption
value of the siliceous solution, stirring speed and stirring paddle position on the sphericity and size of the SAM
was investigated. The SAM with good sphericity was obtained when the pH value was 5.69–5.79. The mean
diameter of the SAM decreased from 5 to 1 mm when the stirring speed increased from 1000 to 2000 rpm. The
SAM with excellent sphericity was prepared when the paddle was placed on the top of the oil bath. When the
paddle was placed at the middle and bottom of the oil bath, some liquid drops aggregated together and formed
large aggregations. AGSAM was obtained by grafting the amine groups onto the framework of the silica gel
microsphere. The CO2 adsorption capacity of the AGSAM was 1.04 mmol g-1 with 1% CO2 at 300 mL min-1. The
AGSAM with 4, 3.2, 2 and 1 mm in diameters had the fluidizing velocities of 0.531, 0.425, 0.265 and 0.159 m s-1,
respectively. The AGSAM with different sizes met different fluidizing conditions.

* Corresponding author. College of Materials Science and Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
** Corresponding author.
E-mail addresses: ykong@njtech.edu.cn (Y. Kong), mfan@uwyo.edu (M. Fan).

https://doi.org/10.1016/j.gce.2020.11.010
Received 8 October 2020; Received in revised form 5 November 2020; Accepted 27 November 2020
Available online xxxx
2666-9528/© 2020 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communication Co. Ltd. This
is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Please cite this article as: X. Jiang et al., Shape-tailorable amine grafted silica aerogel microsphere for CO2 capture, Green Chemical Engineering,
https://doi.org/10.1016/j.gce.2020.11.010
X. Jiang et al.
Fig. 1. The sphericity of the silica gel microspheres with different pH value: (a) the silica gel microspheres with appropriate pH value; (b) the silica gel monoliths with
inappropriate pH value.
1. Introduction
Aerogels are porous materials with interconnected open-pore net-
works constructing of nanoparticles and nanopores, and show unique
structural features including low densities, and large specific surface
areas and nanopore volumes, which endow them with low thermal
conductivities, high sorption capacities, and many other unique features
[1–5]. Therefore, aerogels have excellent performances as thermal in-
sulators, sorbents, catalysts, supports, etc [6–9]. Various aerogels have
been developed, such as oxide aerogels, organic aerogels, carbon aero-
gels, carbide aerogels, biomass aerogels, and so forth [10,11]. Among
these aerogels, silica aerogels were of the greatest attention, and have
realized industrialization and commercialization. In the recent years,
atmospheric CO2 concentrations are increasing at an accelerating rate.
The problem of global warming and climate will become a big trouble to
people's life and study in the near future. Hence, CO2 capture provides an
effective and efficient way to cut the CO2 emissions [12–15]. Recently, it
has attracted intensive attentions to use silica aerogels as CO2 sorbents as
they structure features that can lead to high amine loading [16–18].
Amine functionalized silica aerogels can be finished via wet impregna-
tion, chemical grafting and in-situ synthesis.
The amine functionalized silica aerogels synthesised by Linneen et al.
demonstrated a CO2 adsorption capacity (3.5 mmol g-1, 348 K), attrib-
uted to wet impregnation of tetraethylenepentamine (TEPA) [19,20].
Wang et al. developed a robust silsesquioxane aerogel and impregnated it
with polyetherimide (PEI), the resulting amine functionalized aerogel
exhibited a CO2 adsorption capacity (3.3 mmol g-1, 298 K) [21].
W€ ormeyer et al. developed a silica aerogel by amine grafting and eval-
uated their CO2 adsorption capacity (1.07 mmol g-1, 295 K) [22–24].
Linneen et al. synthesised silica aerogels by wet grafting and showed a
CO2 adsorption capacity (2.61 mmol g-1, 368 K) [25]. By in-situ poly-
merization of amines and siloxanes, Begag et al. prepared amine func-
tionalized silica aerogels. The adsorbents had a CO2 adsorption capacity
in simulated flue gas (1.81 mmol g-1, 277 K) [26]. Kong et al. summarized
a lot of studies on the basis of the in-situ polymerization of APTES and
TEOS. Then, they synthesised amine hybrid silica aerogels and exhibited
high CO2 adsorption capacities (6.66 mmol g-1, 303 K) [27–32].
Although the amine-modified silica aerogels showed excellent CO2
adsorption properties under different circumstances, they are ultralight
powders that cannot be used in the fluidized bed. Hence, these silica
aerogels have to mixed with matrix to form a fixed bed to avoid blockage
[28–30]. Moreover, these silica aerogels were prepared by using silicon
alkoxide and alcohols, which may lead to the increased costs and envi-
ronmental problems in industrialization and commercialization. In this
study, a proof-of-concept CO2 sorbent based on the silica aerogel
microsphere (SAM) was developed for CO2 capture on the fluidized bed
2
Green Chemical Engineering xxx (xxxx) xxx
reactors. A low-cost water glass and environment-friendly water were
used as precursor and solvent of the silica aerogel, respectively. The
siliceous solution silica aerogel was casted to microspheres in different
sizes during the sol-gel process. The effect of the factors that may affect
the sphericity and size of the SAM was investigated. The amine func-
tionalized silica aerogel microsphere was gained by grafting the APTES
onto the framework of the silica gel. The CO2 adsorption property and
fluidized velocity of the amine grafted silica aerogel microsphere
(AGSAM) was investigated.
2. Experimental
2.1. Materials
Water glass (33 wt%, modulus 3.3) used as a precursor was supplied
from the Quechen Silicon Chemical Co., Ltd, China. Acetic acid (AR,
99.5%) used as catalyzer and Dimethicone oil (1000  80 mPa s) were
purchased by the Shanghai Shenbo Chemical Co., Ltd and the Shanghai
Aladdin Biochemical Technology Co., Ltd, China, respectively. APTES
(AR, 98%) as an amine source and Ethanol (EtOH, AR, 99.7%) were
supplied by the Shanghai Aladdin Biochemical Technology Co., Ltd and
the Wuxi City Yasheng Chemical Co., Ltd, China. Deionized water was
home-made.
2.2. Preparation of the SAM and AGSAM
A siliceous solution was formed by mixing Water glass, Water and
Acetic acid with a volumetrical ratio of 6:33:1.2 at 25  C. The SAM was
synthesised by a “ball drop” method. The siliceous solution was dropped
into a hot (70  C) dimethylsilicic oil bath by a syringe pump to form the
silica gel microsphere. The oil bath was rotated at a certain speed by a
mechanical agitator.
The silica gel microsphere was placed in deionized water at 70  C.
The water was changed every 8 h. Then, the silica gel microsphere was
aged with EtOH at 50  C for 2 days. Moreover, an APTES/Ethanol/Water
solution was configurationed with a molar ratio of 1:24:3. The silica gel
microsphere was placed in the solution. The amine grafted silica gel
microsphere was obtained after modification.
The silica gel and amine grafted silica gel was wash with EtOH to
acquire the alcogels. The SAM and AGSAM was obtained after drying the
alcogels with supercritical drying.
2.3. Characterization methods
Apparent density (ρa) was calculated from the weight and the physical
dimensions of the samples. Morphological structures were examined by
X. Jiang et al. Green Chemical Engineering xxx (xxxx) xxx

mechanical stirrer
S ss
drop
siliceous solution
extract oil bath Silica aerogel microspheres

transfer
SCD

syringe pump
water bath

Fig. 2. The flow chart of the preparation of the silica aerogel microspheres.

Fig. 3. The photographs of the SAMs with different stirring speeds: (a) 1000 rpm, (b) 1400 rpm, (c) 1800 rpm, (d) 2000 rpm.

Scanning Electron Microscope (SEM, ZEISS 1530VP). Specific Surface
Area and Pore Size Distribution were characterized by N2 adsorption/
desorption test (BET, Quantachrome Autosorb-iQ analyzer). Fourier
Transform Infrared Spectra (FTIR, Bruker ALPHA) were tested. TG-DTA
curves were implemented by using a thermogravimetric analyzer (TA
instruments SDT Q600). The fluidized velocity was measured with N2 in
a glass tube with inner diameter in 21 mm. The CO2 capture test was
performed on a fixed bed apparatus with a glass tube (21 mm in inner
diameter), which was reported elsewhere [33–35].
3. Results and discussion
3.1. Preparation and shaping of the silica aerogel microspheres
To prepare the silica aerogel microsphere, the gelation kinetics of the
siliceous solution is important. For the water glass-based solution, the pH
value is the key factor that affects the gelation kinetics. Using a simple
“ball drop” method that was conducted by a plastic dropper, it was found
that the silica gel microspheres with good sphericity was obtained when

3
X. Jiang et al. Green Chemical Engineering xxx (xxxx) xxx

Fig. 4. The photographs of the SAMs with different paddles and positions: (a) the paddle on the top of the oil bath; (b) the paddle on the middle and bottom of the
oil bath.

into a hot oil bath by a syringe pump to form the microspheres. It was
found that the stirring speed of the oil bath affected the size of the mi-
50 crospheres significantly. The photographs of the SAMs with different
SAM 1095

AGSAM
stirring speeds were presented in Fig. 3. All the microspheres have good
sphericity and uniform size. The mean diameter of the SAMs decreased
40
from 5 to 1 mm when the stirring speed increased from 1000 to 2000 rpm.
Transmittance, %

The high stirring speed leads to the segmentation of the droplets into
smaller microspheres. The location of the head of the stirring rod also
30
affected the sphericity of the SAMs. Three positions (surface, middle and
bottom of the oil bath) were conducted, the photographs of the SAMs with
different paddles and positions were presented in Fig. 4. The microspheres
20
966
with excellent sphericity was prepared when the paddle was placed on the
1640
top of the oil bath. When the paddle was placed at the middle and bottom
3433 of the oil bath, some liquid drops aggregated together and formed large
10
3500 3000 2500 2000 1500 1000 500 aggregations. The results revealed that the sphericity and size can be
controlled through the stirring speed and position.
Wavenumber/cm-1

Fig. 5. The FT-IR spectra of the SAM and AGSAM. 3.2. Characterizations of the AGSAMs

the pH value was 5.69–5.79. In other cases, the liquid drops clumped
together to form the monoliths, as shown in Fig. 1. It is explained that the
gelation time was 3–5 min when the pH value of the siliceous solution
was 5.69–5.79. Beyond that, it took a longer time to form the gel, leaving
enough time to the liquid drops to aggregate together.
The flow chart of the preparation of the silica aerogel microspheres was
given in Fig. 2. The siliceous solution with pH value of 5.79 was dropped
The AGSAMs were obtained by grafting the APTES onto the silica gel
microspheres. The FT-IR spectra of the SAM and AGSAM were shown in
Fig. 5. The bands around 3433 cm 1 were assigned to the O–H stretching
vibration of the Si–OH groups [36]. The bands at 1640 cm 1 were
attributed to the deformation vibration of the adsorbed water [36]. The
bands at 1095 cm 1 were assigned to the stretching vibration of the
Si–O–Si [36]. The band of the SAM at 966 cm 1 was ascribed to the Si–O
in-plane stretching vibration of the Si–OH groups [36]. For AGSAM, the
band disappeared, owing to the dehydration condensation of hydrolyzed

Fig. 6. The TG and DTA curves of the SAM and AGSAM.

4
X. Jiang et al. Green Chemical Engineering xxx (xxxx) xxx

a b
1600

dv/dlog(W) Pore volume/(cm3 g-1 )

4

SSAM SSAM
1200

Volume/(STP, cm3 g-1 )

SASAM-3 SASAM-3
3

800
2

400
1

0 0
1 10 100
Relative pressure/(P/P0)
Pore width/nm

Fig. 7. (a) N2 adsorption isotherms and (b) pore-size distribution curves of the SAM and AGSAM.

Fig. 8. The SEM images of the SAM and AGSAM.

APTES species and Si–OH groups. As a result, the amine groups are Fig. 6. Weight losses below 134  C were ascribed to the adsorbed CO2 and
grafted by chemical linkage successfully. At the same time, the amine (N) moisture. Weight losses from 134 to 263  C were mianly attributed to the
surface content of the AGSAM from the XPS tests was 3.857 mmol g-1. hydroxy groups. For SAM, weight losses after 263  C were attributed to
The TG and DTA curves of the SAM and AGSAM were depicted in the bonded water and residual hydroxy groups. For AGSAM, the weight
loss at 263  C was assigned to the decompsotion of the –NH2 groups. The

1.2
CO2 adsorption capacity/(mmol g-1 )

0.8

SASAM-3(powder)
SASAM-3(microspheres)

0.4

0.0
0 10 20 30
Time/min

Fig. 9. The CO2 adsorption kinetics of the microsphere and powder samples of
the AGSAM on the fixed bed. Fig. 10. Cyclic CO2 adsorption kinetics of the AGSAM with dry 1% CO2.

5
X. Jiang et al. Green Chemical Engineering xxx (xxxx) xxx

Table 1
CO2 adsorption capacities of AGSAM and its state-of-art counterparts.
Adsorbent Year Apparat Capacity Researcher
(mmol g-1)

AGSAM(microsphere) 2020 Fixed 1.04 This work

bed
AGSAM(powder) 2020 Fixed 1.13 This work
bed
SASA-3 2020 Fixed 1.56 Jiang et al. [35]
bed
SA–I-80 2013 TGA 3.5 Linneen et al.
[19.20]
AFSAS 2012 Fixed 1.07 W€ormeyer et al.
bed [22–24]
AFA 2013 TGA 1.43 Begag et al. [26]
AH-RFSA 2015 Fixed 2.57/5.55/ Kong et al.
bed 6.66 [27–32]

weight loss of the AGSAM after 263  C derived from the decomposition of
the residual –NH2 groups and other organic moities derived from the
APTES. Correspondingly, the endothermic peak at 263  C of the DTA
curve was obserbed. The results demonstrated that the APTES was suc-
cessfully grafted onto the framework of the silica aerogel microsphere.
The N2 adsorption isotherms and pore size distribution curves of the
SAM and AGSAM were observed in Fig. 7. The SAM and AGSAM
exhibited type IV isotherms with H3 hysteresis loops according to the
IUPAC classification, which is the feature of the typical mesoporous
materials [37–39]. There has no more obvious effect of saturation
adsorption in the isotherms of the SAM and AGSAM, reflecting the ex-
istence of the macrospores. The SAM and AGSAM show very similar pore
size distribution, the difference is that the pore volume decreases after
amine grafting. The decrease of the pore volume from SAM and AGSAM
is explained by that the loading of the amine groups block the pore space
to some degree. Hence, the specific surface area and pore volume
decreased from 726 m2 g-1 and 2.27 cm3 g-1 (SAM) to 432 m2 g-1 and
1.78 cm3 g-1 (AGSAM), respectively. The SEM images of the SAM and
AGSAM were shown in Fig. 8. The networks of the aerogels are consti-
tuted by the nanoparticles and nanopores.
3.3. CO2 adsorption performances
Fig. 9 compared the CO2 adsorption kinetics of the microsphere and
powder samples of the AGSAM on the fixed bed. The equilibrium CO2
absorption capacity increases slightly, from 1.04 to 1.13 mmol g-1, after
grinding the microspheres to powders. It suggested that the gas can
diffuse into the AGSAM smoothly, which benefits from the of the inter-
connected network of the AGSAM. This revealed that the AGSAM can be
used for CO2 adsorption directly on the fixed bed and fluidized bed. It
only took 3.85 and 2.4 min to reach 80% of the equilibrium CO2 ab-
sorption capacity of the AGSAM, demonstrating that the AGSAM was a
dynamic adsorbent material for CO2 capture. The cyclic adsorption ca-
pacity of AGSAM with 1% CO2 was described in Fig. 10. The CO2
adsorption property remained unchanged basically through 10 cycles
tests. CO2 adsorption capacities of AGSAM and its state-of-art counter-
parts was shown in Table 1. The microsphere and powder samples of the
AGSAM on the fixed bed shown good CO2 adsorption capacities.
The use of the AGSAM in the fluidized bed was developed. The
Fig. 11. Effect of flow velocity on CO2 sorption capacity of the AGSAM with dry
1% CO2 (the AGSAM samples with different sizes on the fluidized bed; the
microsphere samples of the AGSAM on the fixed bed; the powder samples of the
AGSAM on the fixed bed).
fluidizing velocities of the AGSAM samples with different sizes were
shown in Table 2. The AGSAM samples with 4, 3.2, 2 and 1 mm in di-
ameters have the fluidizing velocities of 0.531, 0.425, 0.265 and 0.159 m
s-1, respectively. It reveals that the shape and size-tailorable AGSAM can
meet different fluidizing conditions.
The CO2 adsorption capacity of the AGSAM in the fluidized bed can
be investigated. The CO2 adsorption capacity of the AGSAM samples with
different sizes were described in Table 2. Under certain conditions, the
CO2 adsorption capacity of AGSAM decreases with the increase of the gas
velocities [40]. When the fluidizing velocities decrease from 0.531 m s-1
to 0.159 m s-1, CO2 adsorption capacities of AGSAM increase from 0.17 to
1.08 mmol g-1. The result was also basically consistent with our previous
research conclusions on CO2 adsorption performance in fixed bed [32].
The effect of flow velocities on CO2 sorption capacity of the AGSAM with
dry 1% CO2 was observed in Fig. 11. The CO2 adsorption capacities of the
AGSAM with different sizes show a linear relationship at different flow
rates. The amine grafted silica aerogel microsphere exhibits similar
adsorption capacities to powdered aerogels due to their unique shape
advantages. It indicated that the AGSAM samples with different sizes can
be used as a sorbent on the fluidized bed.
4. Conclusions
A silica aerogel microsphere was developed by a low-cost and
environment-friendly “ball drop” method. The sphericity and size of the
silica aerogel microsphere was regulable through changing the pH value
of the siliceous solution, the stirring speed and the stirring paddle posi-
tion in the coagulating bath. Amine grafted silica aerogel microsphere
was obtained by grafting the APTES onto the framework of the silica gel.
The amine grafted silica aerogel microsphere showed high CO2

Table 2
The fluidizing velocities and CO2 adsorption capacity of the AGSAM samples with different sizes.
Samples Density/(g cm-3) Particle size/(mm) Flow velocity/(m s-1) CO2 adsorption capacity/(mmol g-1)

AGSAM 0.024 4 0.531 0.17

0.023 3.2 0.425 0.43
0.022 2 0.265 0.82
0.021 1 0.159 1.08

6
X. Jiang et al.
adsorption activity. The amine grafted silica aerogel microsphere was
available on both fixed bed and fluidized bed. The amine grafted silica
aerogel microsphere samples with different sizes can meet different
fluidizing conditions. In conclusion, the sorbent preparation method is
simple, cost-effective and environment-friendly, the resulting adsorbent
is dynamic and can be directly used as a CO2 capture on both fixed and
fluidized beds.
Declaration of competing interests
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgment
The authors acknowledge the supports from the National Natural
Science Foundation of China (51602151), the Natural Science Founda-
tion of Jiangsu Province - China (BK20161003), the Project funded by
China Postdoctoral Science Foundation (2018T110490, 2018M642228),
and the Priority Academic Program Development of Jiangsu Higher Ed-
ucation Institution (PAPD) - China. The authors would like to thank
Shiyanjia Lab (www.shiyanjia.com) for the support of BET test.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.gce.2020.11.010.
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