Materials & Design 130 (2017) 452–458

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Materials & Design

journal homepage: www.elsevier.com/locate/matdes

Cotton aerogels and cotton-cellulose aerogels from environmental waste for MARK
oil spillage cleanup
Hanlin Cheng, Bowen Gu, Mark P. Pennefather, Thanh X. Nguyen, Nhan Phan-Thien,
Hai M. Duong⁎
Department of Mechanical Engineering, National University of Singapore, 9 Engineering Drive 1, EA-07-08, 117575, Singapore

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

Keywords: For the first time, successful fabrication of the cotton aerogels and cotton-cellulose aerogels is achieved using
Cotton fibers recycled fibers from environmental waste for oil absorption. The pure cotton and cotton-cellulose aerogels are
Cellulose fibers obtained using a cost-effective mixing-blending method with polyamide-epichlorohydrin as strengthening
Aerogel additives. The obtained aerogels are silanized using methyltrimethoxysilane via a facile chemical vapor
Oil absorption
deposition to endow aerogels with hydrophobic surface. Effects of fiber concentrations and cotton-to-cellulose
Environmental waste
mass ratio on oil absorption performance in various solvents are also investigated. The cotton aerogel with an
initial concentration of 0.25 wt% presents the highest oil absorption capacity over 100 g g− 1. Besides, the
cotton/cellulose aerogels also demonstrate good absorption capacity in different pollutant organics. The
absorption kinetics of the aerogels with different cotton concentrations are also investigated using pseudo
first-order model. Both equilibrium absorption and absorption kinetics demonstrate cotton/cellulose aerogels as
promising materials for oil absorption and environmental pollution treatment.

G RA P H I C A L AB S T R A C T

1. Introduction ecology system. To date, various technologies including chemical

Oil removal and separation are becoming important due to acci-
dental oil leakage and oil spillage from the ever-increasing oil industry.
The untreated oil waste and contaminant not only cause the unneces-
sary economic loss but are dangerous to the environment and the
treatments [1], bioremediation [2,3] and physical skimming [4–6]
have been developed for the oil absorption and separation. Among
these methods, using absorbents to directly remove the oil from the
contaminated area is the most efficient and cost-effective [7–9]. More-
over, it also brings great convenience if the absorbed oil can be recycled

⁎
Corresponding author.
E-mail address: mpedhm@nus.edu.sg (H.M. Duong).

http://dx.doi.org/10.1016/j.matdes.2017.05.082
Received 19 February 2017; Received in revised form 26 May 2017; Accepted 27 May 2017
Available online 28 May 2017
0264-1275/ © 2017 Elsevier Ltd. All rights reserved.
H. Cheng et al. Materials & Design 130 (2017) 452–458

upon simple squeezing [10], distillation [11] or extraction [12]. Table 1

Commercial sorbents including polypropylene mats with remark- Properties of pure cotton (PC) and cotton-cellulose (CC) aerogels with different cotton
able hydrophobicity and oil absorption capacity of 15 g g− 1 [13] have concentrations and cotton-cellulose mass ratios.

been widely used in the oil pollutant treatment. Additionally, other Aerogels Concentration (wt Mass ratios of Density Porosity (%)
synthetic polymers such as polypyrrole sponge [14], polyurethane [15], %) cotton-cellulose (mg cm− 3)
polydimethylsiloxane [16], and polysiloxane [17] have been used for
PC25 0.25 1:0 5.13 ± 0.29 99.66
the oil absorption. However, their applications are greatly limited not
PC50 0.50 1:0 6.85 ± 0.33 99.54
only because of their low absorption capacity but also their poor PC75 0.75 1:0 8.22 ± 0.49 99.45
environmental compatibility [13]. The synthetic polymers stay long CC1-1 0.50 1:1 8.50 ± 0.33 99.43
time in environment due to its difficulty to degrade and their CC1-2 0.50 1:2 6.40 ± 0.08 99.57
accumulation in the ecosystem makes this problem more serious [18]. CC1-4 0.50 1:4 6.19 ± 0.33 99.59

To further improve the oil absorption capacity, nano-designed carbon

materials have been developed [19–21]. Carbon nanotube sponge
2. Experimental section
derived from the chemical vapor deposition method (CVD) can achieve
an ultrahigh absorption capacity of 120 g g− 1 with remarkable me-
2.1. Materials
chanical reversibility [20]. Ultralight graphene aerogel with an absorp-
tion capacity of 200 g g− 1 in chloroform was also used for the
Recycled cellulose fibers from paper waste and polyamide-epichlor-
contaminant absorption [21]. Although pure cotton fibers suffer a
ohydrin (PAE, Kymene 557H) were obtained from Insul-Dek
low capacity below 30 g g− 1 [22], a high temperature pyrolysis can
Engineering Pte. Ltd. (Singapore) and Ashland (Taiwan), respectively.
convert commercial cottons directly to carbon foam with good mechan-
The cotton pads consisting of cotton fibers were purchased in the
ical stability for oil absorption applications [23]. However, this high
Fairprice (Singapore). Motor oil (5w40) and Singer machine oil were
temperature treatment and the small-scale production make them cost
purchased from commercial market. Analytical grade MTMS, ethanol,
inefficient for oil removal applications [24]. Besides, the carbon
acetone, hexane and dichloromethane were obtained from the Sigma-
nanomaterials are not bio-degradable and may cause potential health
Aldrich (Singapore). All chemicals were used without further purifica-
issues [25,26].
tion.
In order to overcome these challenges, great effort has been focused
on cellulose derived materials due to its rich natural abundance and
2.2. Synthesis of pure-cotton (PC) and cotton-cellulose (CC) aerogels
environmental benignity [27–29]. Unlike synthetic polymers and nano-
carbon materials, cellulose can be easily decomposed by certain
The synthesis process of the PC and CC aerogels is illustrated in
bacterial in environment [30]. Methods such as oleophilic TiO2 coating
Fig. 1. The cotton pads were cut into small strands (0.5 × 4 cm) and
[28] and silanization routine using methyltrimethoxysilane (MTMS)
then were mixed with the cellulose fibers recycled from the paper waste
[29] can functionalize cellulose fibers with hydrophobic surface to
in 200 ml deionized water. The cotton-to-cellulose mass ratios were
render them good candidates for oil absorption. Among different types
fixed at 1:0 (pure cotton), 1:1, 1:2 and 1:4 and the fiber-to-water mass
of cellulose [8,20–23], nanocellulose-based products have achieved
concentration in aqueous dispersion was controlled with 0.25 wt%,
high adsorption capacity [10,31]. However, the fabrication process of
0.5 wt% and 0.75 wt%, respectively Then, the mixture dispersion was
nanocellulose is expensive and time-consuming. To understand the oil
homogenized using a juice blender (Tefal 400W) for 15 min. After-
absorption process, various models have been proposed [32–34] for
wards, 66.6 μL PAE solution was added into the above dispersion,
kinetics calculation. Among them pseudo-first model is widely used for
which later went through a sonication process (Hielscher Ultrasound
the oil absorption [35].
Technology) at 140 W for 5 min. The homogenized dispersion was
To reduce the environmental burden and establish green production
frozen at − 18 °C for 24 h and then dried in vacuum at −98 °C for 96 h
recycle, investigations on cellulose absorbent from waste paper have
to obtain the monolith aerogels. During the freeze, both cotton and
been reported in our previous research [36,37]. It was found that the oil
cellulose fiber was squeezed due to the volume expansion from water to
absorption capacity was merely around 50 g g− 1. The further increase
ice. Finally, these aerogels were cured at 120 °C for another 3 h.
of the oil absorption capacity by reducing the material density
inevitably leads to the poor mechanical performance. Meanwhile,
cotton is a commercial available cellulose based material, which is 2.3. Hydrophobic functionalization of the aerogels
cost-effective and environmental friendly. Its packed cellulose structure
is believed to increase the stability of the aerogels. Therefore, in this In order to obtain the hydrophobic aerogels for oil absorption, the
work, we successfully develop pure cotton (PC) and cotton/cellulose obtained aerogels were placed in the glass chamber with four poly-
(CC) aerogels from the paper waste for the oil absorption application tetrafluoroethylene vials with each containing 1.5 ml MTMS and heated
with good absorption capacity and mechanical handleability. at 70 °C for 12 h to undergo a silanization process. The silanization
process was carried out based on the reaction between hydroxyl groups
and alkoxy groups in MTMS [38]. The PC aerogels were prepared using

Fig. 1. Schematic illustration of the synthesis of PC and CC aerogels.

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H. Cheng et al.
the same method without the addition of the cellulose fibers. The PC
aerogels with different fiber-to-water concentrations and the CC aero-
gels with different cotton-to-cellulose mass ratios are summarized in
Table 1, where the parameters changed are marked with bold font.
2.4. Characterizations
Sample morphologies were investigated by a scanning electron
microscope (SEM, JSM-6010 of Japan). Before the testing, samples
were sputtered with a thin layer gold via JEOL sputter (JFC-1200) at
20 mA for 30 s to enhance their electrical conductivity.
Sample weight was measured by a digital microbalance with
accuracy of 0.01 mg. Water contact angles measurements were carried
using a syringe system (VCA Optima goniometer, AST Products Inc.
USA) with each droplet of 0.5 μL. The bulk density of the samples was
obtained by measuring the mass and volume of the cylinder-shaped
aerogels. The porosity, Φ, can be calculated by:
⎛ ρ⎞
ϕ = 100 ⎜1 − a ⎟
⎝ ρc ⎠
Where ρa is the density of the aerogel and ρc (1.5 g cm− 3) is the density
for both cellulose and cotton fiber since they process similar density
[37,39].
Equilibrium oil and water absorption tests were also conducted.
Each sample (~ 10 mg) was immersed into the certain oil or water for
30 min to reach the equilibrium and then was drained for another
20 min to determine the weight. The absorption capability can be
calculated by:
m w − md
Qr =
md
Where Qr (g g− 1) is the absorption capability, md (g) and mw (g) are the
aerogel weight before and after the oil absorption, respectively. The
error range including the standard deviation was determined by the
Analysis of Variance in software “Originlab”.
To determine the oil absorption kinetics, samples with identical size
(cylinder shape with diameter of 6 cm and height of 3 cm) was
immersed into the singer machine oil at different time to measure its
weight change. The kinetic constant, k1 was determined by [40]:
Qm
ln = k1 t
Qm − Qt
Where Qmis the saturated absorption capacity (g g− 1), Qtis the absorp-
tion capacity (g g− 1) at time t (s).
For the distillation absorption cycling experiment, after the absorp-
tion of ethanol, aerogels were placed into a flask and heated at 100 °C
with a condenser to collect the recycled ethanol. For the squeezing
absorption cycling experiment, after the absorption of ethanol, the
aerogel was squeezed to one fourth of height original to release the
ethanol.
Fig. 2. (a) A large-scale CC1-1 aerogel, (b) The CC1-1 aerogel can stand an empty 100 ml beaker (~53 g) place on the top, and (c) MTMS-coated CC1-1 aerogel does not absorb blue water
droplets.
Materials & Design 130 (2017) 452–458
3. Results and discussion
The PC and CC aerogels possess good handleability. Various shape
and size of the developed aerogels can be controlled using molding.
Fig. 2a shows a large-scale CC aerogel having 1-cm thickness, 0.50 wt%
and the cotton-cellulose ratio of 1-1 can be fabricated using the A4-
sized tray. The good handleability of the CC aerogel can be found with a
height change less than 80% when placing a 100 ml glass beaker
weighted ~53 g, which is near 100 times of aerogel (Fig. 2b). Fig. 2c
exhibits the MTMS-coated CC aerogel does not absorb small water
droplets (dyed with blue ink) placed on its top surface, confirming its
hydrophobicity.
The results of water contact angle tests of different PC and CC
aerogels are shown in Fig. 3. A large contact angle over 130° of all PC
and CC aerogels indicates their hydrophobic properties. The contact
angle slightly decreases with the increase of the cotton concentration.
This occurs because the homogenous silanization process may be less
effective. Compared with the 0.50 wt% PC aerogel, the CC aerogels
with the same 0.50 wt% have a larger contact angle up to 142.8o. It can
be explained that more cellulose fibers can add more hydroxyl groups
(1) exposed to the MTMS vapor, which are replaced by the alkoxy groups
and make surface of the CC aerogel more hydrophobic [41,42]. The
further increase of cellulose content also brings the decrease of the
water contact angle, possibly due to a less-efficient coating. Although
some reports achieved superhydrophobic cellulose with constant angle
above 150 °C, our work has merit of a low-cost raw materials and
simple functionalization method [43–45].
The PC and CC aerogels present macropores with diameter larger
than 50 μm estimated from the SEM images in Fig. 4. For the PC
aerogels, the increase of the cotton fiber concentration causes more
packed structure as seen in Fig. 4a–c. For the CC aerogels in Fig. 4d–f,
(2) the increase of the cellulose fibers also causes more packed structure. It
may be explained that the cellulose fibers can be dispersed better than
the cotton fibers. The SEM image of the MTMS-coated CC aerogel is
presented in Fig. S1 (Data in Brief) and there is no apparent morphology
difference between the uncoated samples due to the very small amount
of MTMS usage.
Fig. 5 demonstrates the absorption process of machine oil (dyed
using Sudan Red) using the CC1-1 aerogel with the size of
2 × 2 × 0.5 cm. The aerogel initially floats on the oil and then
gradually sinks down upon the absorption of the oil. The absorption
is completed in 180 s. Besides, the CC aerogels can be shaped into small
(3) pellets to treat and remove the oil from the water as shown in the movie
S1. The aerogel pellets can help on storage space reduction and easy
transportation.
Fig. 6 exhibits the machine oil absorption capabilities of the PC and
CC aerogels. Samples with different fiber concentration clearly show
different absorption performance analyzed by F-test using one-way
Anova. As can be seen in Fig. 6a, the PC aerogel with a low
concentration of 0.25 wt% has the highest absorption capacity over
100 g g− 1, much larger than those of the commercial sorbents. The
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Fig. 3. Contact angles of the MTMS-coated PC aerogels with different concentrations: (a) PC25, (b) PC50, (c) PC75 of the cotton fibers and MTMS-coated CC aerogels having the same
0.50 wt% of the fibers with different cotton-cellulose ratios: (d) CC1-1, (e) CC1-2, and (f) CC1-4.

increase of the cotton fiber concentration from 0.25 wt% to 0.75 wt%
decreases the absorption capability of the PC aerogels due to their
raised density and lower porosity as listed in Table 1. For the CC
aerogels in Fig. 6b, both CC1-1 and CC1-2 aerogels present competitive
oil absorption compared to the PC aerogel with same fiber concentra-
tion of 0.50 wt%. It is also important to note that during the draining
period to remove the oil absorbed, the CC aerogels show little shape
change while the PC aerogel shrink to the 80% of the original volume.
This provides an indirect evidence of the better mechanical stability of
the composite design over the pure cotton aerogel. With the further
increase of the cellulose fibers leads to the decrease of the absorption
capability despite of its smaller density. Two reasons can be used for
explanation: (i) the dense structure in Fig. 4f can prevent the oil
diffusion and entrap the great air inside the aerogels, (ii) the higher
percentage of the cellulose fiber leads to an inefficient silanization
process due to more exposed hydroxy groups while the amount of
MTMS used for coating is fixed [46].
Water absorption capability of the MTMS-uncoated PC and CC
aerogels are illustrated in the Fig. S2 (Data in Brief). Interestingly, we
find that although the water absorption capacity of PC aerogels is much
higher than our previous pure cellulose aerogel (~ 20 g g− 1) [37], it is
much smaller than the absorption capacity of machine oil, regardless of
the larger density of the water. Both cotton aerogels and cotton/
cellulose aerogel were swelled during the water absorption tests.
However only cotton aerogels were swelled during the oil absorption
tests. Also, it is found that during the draining process after the water
absorption capability, the prepared cotton aerogels undergo an ob-
servable shrink (~ 60% volume change) once taken out from the water.
Meanwhile this volume shrinkage is much smaller in the oil absorption
tests. This can be explained by the high viscosity of the machine oil
compared with the water. It is worth noting that this difference is much
smaller in the CC aerogels, indicating their improved mechanical
strength. Although some reports [23,28] have achieved higher absorp-
tion values, they either suffer a complex fabrication process using
nanocellulose [31] or an environmental hazardous pyrolysis process
[23].
The absorption kinetic results are shown in the Fig. 6c. The PC50
aerogel has the highest absorption speed compared with the CC
aerogels. But the CC1-4 aerogel has the lowest absorption capability
and the sluggish absorption kinetic, possibly due to its least hydro-
phobicity. The initial absorption kinetic constants are obtained by
fitting the results according to the notable first-order pseudo Eq. (3).
The kinetic constants of the PC50, CC1-1, CC1-2, and CC1-4 aerogels in
Fig. S3. (Data in Brief) are 0.217, 0.094, 0.143 and 0.189, respectively.

200 µm

Fig. 4. FESEM images of the PC aerogels with different concentrations of (a) PC25, (b) PC50, (c) PC75 and the CC aerogels with different cotton-cellulose ratios of (d) CC1-1 (e) CC1-2, (f)
CC1-4.

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Fig. 5. Oil absorption process of the CC1-1 aerogel in 180 s.

Fig. 6. Machine oil absorption capacities of (a) the PC aerogels with different cotton fiber concentrations (0.25–0.75 wt%), (b) CC aerogels with different cotton-cellulose ratios (1-1 to 1-
4), and (c) absorption kinetics of PC50 aerogel and CC aerogels with different cotton-cellulose ratios (Figure inset is the absorption result in initial 30 s with fitting lines).

Fig. 7. Various solvent absorption capacity of the (a) CC1-1 aerogel and (b) absorption capacity marked with liquid density.

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Fig. 8. Distillation cycling of (a) the PC50 aerogel and (b) the CC1-1 aerogel for ethanol absorption.
Besides the machine oil, the aerogels are also tested with other
organic solvents. As can be seen in the Fig. 7, the CC1-1 aerogel
presents the highest absorption capacity for dichloromethane and the
least for hexane. Generally, the absorption capacity increases with the
density of the solvent. However, the absorption capacity for the acetone
is higher than that for the ethanol regardless of their close density
(Fig. 7b). The absorption capacities of the PC and CC aerogels
developed in this work are higher than those of conjugated polymers
[24], nanowire membrane [47], exfoliated graphite [48], carbon
aerogel [49] and competitive to spongy CNT and graphene [50,51].
We also plot the theoretical absorption ratio based on the solvent
density and sample porosity (porosity × ρliquid / ρaerogel). Current ab-
sorption capacities of the CC1-1 aerogels for the different solvents are
near the line of the theoretical absorption capacity. It is believed with
increased pressure, higher absorption capacity can be achieved.
More importantly, the absorbed liquids can be re-collected through
the distillation. Fig. 8 shows the absorption-distillation cycles of the
ethanol. Both PC50 and CC1-1 aerogels undergo minor shrinkage
during the distillation process due to the capillary force during the
liquid-vapor phase transition [52]. After 5 cycles of liquid recovery, the
PC50 and CC1-1 aerogels yield the absorption capacities of 38 ad
40 g g− 1, respectively. The CC1-1 aerogel presents a slightly better
performance because the strengthening effects of two different cotton
and cellulose fibers [53]. Compared with the poor absorption cycling
capacity in squeeze-cycling method (Fig. S4, Data in Brief), the
distillation method clearly presents a better performance.
4. Conclusions
In summary, we have successfully prepared the cotton/cellulose
composite aerogels using commercial cotton and cellulose fiber from
paper waster. The functionalized aerogels with hydrophobicity demon-
strate a good contaminant absorption with 72.3 g g− 1 in machine oil
and 94.3 g g− 1 for dichloromethane. The cotton/cellulose composite
aerogel presents a slightly better performance because the synergistic
effects of two different cotton and cellulose fibers.
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.matdes.2017.05.082.
Acknowledgement
We'd like to thanks FB Fund C-265-000-049-001 for the funding
support and the lab officers in Materials Division, Department of
Mechanical Engineering, NUS for their significant help on characteriza-
tions.
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