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A novel method to prepare water-soluble core

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Cite this: Polym. Chem., 2014, 5,

microcapsules with controlled burst release
6060
Mingming Zuo, Tianqing Liu* and Jingjing Han

Received 4th May 2014,
Accepted 16th June 2014
DOI: 10.1039/c4py00616j
www.rsc.org/polymers
The controlled burst release of water-soluble materials from microcapsules is very important in many
practical applications. A novel method is described to synthesize microcapsules containing water-soluble
materials, ammonium persulfate or sodium nitrite, as the core and a hydrophobic copolymer (P(St–MMA))
as the shell through an evaporation–dispersion–polymerization process. The microcapsules had an
average size of 8–16 μm. The release behavior was examined at different temperatures, pH values and
salinities. The release pattern of the cores from the microcapsules was burst release. After a given time
period in the 10–45 h region, all of the cores could be completely released within 1 h from the micro-
capsules. The structures, dispersion and morphologies of the microcapsules were characterized before
and after they were stored for 5 months at room temperature. This method further enhances the potential
of microcapsules with burst release properties for practical applications.

1. Introduction
Microcapsules have great potential for applications which
involve encapsulating and releasing various kinds of active
substances,1 such as drugs, enzymes, food additives, cells, and
other things.2–12 The controlled release of core materials
encapsulated in microcapsules can be achieved under the
influence of certain factors.13 So far, a variety of chemical or
physical methods have been developed for the preparation of
microcapsules with water-soluble cores, such as microfluidic
techniques,14,15 self-assembly,16,17 precipitation,18 template-
mediated interfacial reactions,19 spray-drying,20 and a promis-
ing in situ polymerization technique.21,22 However, core
materials in microcapsules synthesized through these encap-
sulation methods can only be slow-release controlled; i.e. the
encapsulated core materials can not achieve the result of burst
release at a given time.
The controlled burst release of encapsulated water-soluble
materials is of considerable significance in many fields. For
example, ammonium persulfate (APS), a general oilfield gel
breaker, can undergo controlled burst release from microcap-
sules to solve the problem of the premature decrease in the
fracturing fluid’s viscosity during its construction period.23,24
Thus the fracturing construction period can be prolonged and
the amount of tertiary oil recovery is also improved in the oil-
field. Ammonium polyphosphate, an excellent flame retardant
material for epoxy resin, can be encapsulated and subjected to
controlled burst release. The burst release properties not only
improve the epoxy resin thermal stability and flame retar-
dancy, but also extend its service life.21 Water-soluble anti-
cancer drugs can undergo controlled burst release from
microcapsules to ensure that the drugs are delivered to the
designated location at a controlled relevant concentration.15
The controlled burst release of a corrosion inhibitor (sodium
nitrite) can control the release time and keep the properties
unchanged before it reaches an intended position.25 Effectively
encapsulating water-soluble materials into microcapsules and
making them burst release is still a very important and chal-
lenging issue.
In this paper, we present a novel evaporation–dispersion–
polymerization method to prepare microcapsules composed of
water-soluble cores (APS or sodium nitrite). The water-soluble
cores can be subjected to controlled burst release from the pre-
pared microcapsules at a given time in the 10–45 h region after
the microcapsules are placed in a medium, and are completely
released within 1 h. In addition, we also encapsulated water-
soluble sodium nitrite into the microcapsules effectively using
this method and it can also be subjected to controlled burst
release. The general method can be readily extended to prepare
diverse microcapsules with many other water-soluble materials,
such as water-soluble drugs and phase-change materials.
2. Experimental section
Materials

School of Chemistry and Chemical Engineering, Yangzhou University, Analytical grade ammonium persulfate (APS) (ground in a
Yangzhou 225002, P. R. China. E-mail: tqliu@yzu.edu.cn; Tel: +86-514-87975590-9517 mortar before use), polyoxyethylene sorbitan monooleate

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Polymer Chemistry
(Tween 80), dichloromethane, n-hexane, stearic acid, polyvinyl-
pyrrolidone (PVP, average molecular weight 1.3 × 106), and 2,2′-
azobis(2-methylpropionitrile) (AIBN) were all purchased from
Sinopharm Chemical Reagent Co. Ltd, China. Technical grade
monomers of styrene (St) and methyl methacrylate (MMA)
were distilled under vacuum to remove trace amount of inhibi-
tors ( purchased from Guangzhou Langri Chemical Co. Ltd,
China.) just prior to use. The water used in all treatment pro-
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cesses was deionized by a milli-Q Plus system (Millipore,
France), with 18.2 MΩ electrical resistivity.
Synthesis of the microcapsules
The standard core/shell microcapsules used in this work were
synthesized via an evaporation–dispersion–polymerization
method, which is described as follows. ‘A’ phase was formu-
lated by adding the following components into an n-hexane
solution (85 mL): Tween 80 (0.30 wt%) and APS (5 wt%). The
mixture was warmed up to 40 °C and stirred (100 rpm) for
1.5 h. ‘B’ phase (25 mL) consisted of dichloromethane
(15 mL), stearic acid (0.1 g) and monomers (the weight ratio of
St and MMA was 40 : 60). The two phases were mixed, and
then they were warmed up to 70 °C and stirred for about 3.5 h.
Following this procedure, PVP (0.1 wt%) and AIBN (0.15 wt%
of monomer) were added, and the mixture was stirred for
another 4 h until the dichloromethane had evaporated com-
pletely and the monomers were consumed. The obtained pro-
ducts were dried at 50 °C under vacuum after washing with
n-hexane once and distilled water twice to remove residual
monomers, emulsifiers and solvents.
Characterization
Scanning electron microscope (SEM) photographs of dried
microcapsules coated with a thin layer (about 15–20 nm) of
gold were taken using a field emission scanning electron
microscope (FE-SEM, S-4800, Japan). The morphologies of the
microcapsules were examined by a transmission electron
microscope (TEM, TECNAI-12, Philips, Netherlands) and an
optical microscope (OM, DMLP, Germany). The samples were
dispersed by ultrasonication in distilled water. The size distri-
bution and diameters of the microcapsules were determined
using dynamic light-scattering on a Zetasizer Nano ZS-90 (DLS,
Malvern Instruments, England). A dispersion of the microcap-
sules was diluted up to 30 times with distilled water for the
analysis. Fourier transform infrared (FTIR) spectra of the
samples were recorded in the range 400–4000 cm−1 using FTIR
spectroscopy (Nicolet-740, United States). The sample was pre-
pared by grinding with spectroscopic-grade potassium
bromide (KBr). The X-ray diffraction (XRD) patterns of the
samples were recorded on a German Bruker AXS D8 ADVANCE
X-ray diffractometer. The thermal analysis was performed
using a NETZSCH STA 409PC thermogravimeter (TGA,
Germany). The temperature was increased from 10 to 800 °C
with a temperature increase rate of 10 °C min−1 under a nitro-
gen atmosphere. The release profile of APS from the microcap-
sules was monitored by a conductivity meter (DDS-11A,
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Shanghai Weiye Corporation, China) at different temperatures,
pH values, and salinities.
3. Results and discussion
Morphology and size distribution of the microcapsules
Fig. 1 shows some SEM, TEM and size distribution images
taken in the formation process of the APS core/shell microcap-
sules. As shown in Fig. 1a and b, the microcapsules were aggre-
gated in the n-hexane/dichloromethane/Tween 80/monomers
(St and MMA) system. Here the microcapsules were connected
to each other by a polymeric substance because the generated
copolymer was soluble in dichloromethane.26 The average
maximum diameter reached up to 50–70 μm (Fig. 1c). When
an appropriate PVP content was added, the aggregation
phenomenon weakened (Fig. 1d and 1e), the average diameter
decreased (within 20–40 μm) and the size distribution of the
microcapsules became narrow (Fig. 1f ).
After the dichloromethane was completely removed, the
adjacent microcapsules were connection-free and were distinct
core–shell structures with shell thicknesses of 2–5 μm (Fig. 1g
and 1h). The diameter of the microcapsules decreased (mainly
8–16 μm) and the size distribution appeared more narrow
(Fig. 1i). A schematic formation process of the microcapsules
prepared through evaporation–dispersion–polymerization is
illustrated in Fig. 1j. The monomers (St + MMA) were initiated
at 70 °C by APS dispersed in the n-hexane/dichloromethane/
Tween 80/PVP system to form a copolymer, which was dis-
solved in dichloromethane. Thus, the APS surface was coated
by a uniform and compact copolymer shell. When dichloro-
methane volatilized completely, the copolymer dissolved in the
dichloromethane separated out to adhere onto the APS sur-
faces to form core/shell APS microcapsules with controlled
burst release properties.
Components and thermal stability of the microcapsules
The composition of the APS microcapsules was characterized
by FTIR and XRD (Fig. 2). The characteristic absorption bands
of APS appear at 1060, 1400 and 3180 cm−1, which are
assigned to the sulfate group and a stretching vibration (νN–
H). These APS bands existed in the spectra of the APS micro-
capsules (Fig. 2a). The characteristic absorption bands of P(St–
MMA) all appeared in the spectra of the microcapsules. The
bands at 750 and 845 cm−1 are assigned to flexural vibrations
(δC–H) of the benzene ring in polystyrene.27 The peaks at 2924
and 2852 cm−1 are the absorption bands of the C–H
vibrational modes in methyl and methylene. The band at
1733 cm−1 corresponds to a carbonyl stretch vibration of
poly(methyl methacrylate).28,29
In Fig. 2b, the main XRD pattern peaks of the APS micro-
capsules are consistent with that of pure APS, which also
indicates the presence of APS in the microcapsules. Due to
the amorphous characteristics of P(St–MMA), there was no
obvious polymer diffraction peaks in the microcapsules.
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Fig. 1 (a, d, g) FE-SEM, (b, e, h) TEM, and (c, f, i) diameter and size distribution images of the APS microcapsules synthesized with (a, b, c) emulsifier
(Tween 80) in dichloromethane–n-hexane solution, (d, e, f ) emulsifiers (Tween 80 and PVP) in dichloromethane–n-hexane solution, and (g, h, i)
emulsifiers (Tween 80 and PVP) in n-hexane solution. Scale bar is 50 μm. Insets show corresponding magnified FE-SEM and TEM photographs
(scale bar is 10 μm). ( j) Schematic formation process of the microcapsules.

Fig. 2c and d show the TGA and DTG curves of the APS and
APS microcapsules. The weight losses of 6.24% and 6.34% at
201 °C are due to the evaporation of physically adsorbed water
in APS and the microcapsules, respectively. For the microcap-
sules, the thermal degradation curve can be divided into three
steps. The weight loss of 34.3% between 201–340 °C, which is
attributed to the removal of the polymer shell, indicates the
formation of the copolymer initiated by APS. Based on the cal-
culation results obtained, the residual weight of 48.5% should
be the APS weight.28 This shows that the content of APS

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Fig. 2 FTIR spectra (a), XRD pattern (b), TGA (c), and DTG (d) curves for both the APS and APS microcapsules (MCc).
encapsulated in the microcapsules reached 48.5% and the
decomposition temperature of APS increased obviously.
Shell surface analyze of microcapsules
The FE-SEM photographs of the shell surface of the microcap-
sules obviously reveal an exterior coated with 50–100 nm nano-
particles, which are highly compacted with each other (Fig. 3).
This may be explained by the fact that the monomers (St–
MMA) are firstly dispersed as droplets as an effect of the emul-
sifiers (Fig. 4b). With the evaporation of dichloromethane, the
droplets are adsorbed on the APS surfaces (Fig. 4c). Finally,
they are initiated by APS and AIBN to form the shell materials
of the microcapsules (Fig. 4d). When the dichloromethane
Fig. 3 (a) Low-magnification and (b) high-magnification FE-SEM
photographs of a single microcapsule synthesized in dichloromethane–
n-hexane solution.
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evaporates completely, the excess droplets are initiated by
AIBN to form polymeric microspheres and coat on the exterior
surface (Fig. 4e).
Controlled release of APS from the microcapsules
Some simulated conditions are presented to evaluate the con-
trolled release behavior of the microcapsules. Fig. 5 shows the
effect of temperature, pH, and NaCl concentration on the
release time of APS from the microcapsules.
P(St–MMA) has swelling properties in water. The release of
APS from the microcapsules depends on the swelling and frac-
tures of the copolymer. With the increase of temperature, the
swelling degree and the permeation ability of water through
the P(St–MMA) shell all increased. The swelling and the per-
meation amount was large enough to lead to the rupture of
the P(St–MMA) shell, and APS was completely released from
the microcapsules within a controllable time (Fig. 5a). The
burst release time is normally not controlled by pH (Fig. 5b)
because P(St–MMA) is a pH-unresponsive amorphous thermo-
plastic copolymer.30 Increases in NaCl concentration can
enhance the ionic strength, which results in a decrease in the
swelling degree of the P(St–MMA) shell and the permeation
ability of water from the outside into the microcapsules is
also restrained.31 The release time slightly increased as the
NaCl concentration increased (Fig. 5c). The swell and rupture
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Fig. 4 Formation mechanism of the exterior surface of the APS microcapsules coated with 50–100 nm nanoparticles.

Fig. 5 Controlled release behavior of the encapsulated APS monitored by a conductivity meter. Relationship of the burst release time of APS from
the microcapsules with (a) temperature at pH 7.0 and [NaCl] 100 mg L−1; (b) pH at 70 °C and [NaCl] 100 mg L−1; and (c) NaCl concentration at
pH 7.0 and 70 °C. (d) The swell and rupture mechanism of the APS microcapsules in water. Other conditions: 1% w/w APS microcapsules were
added to 100 mL distilled water.

mechanism of the P(St–MMA) shell of the microcapsules is The thickness (data in Fig. 6) of the copolymer shell of the
shown in Fig. 5d. microcapsules increased from 0.8 μm to 2.9 μm with the
Fig. 6A shows TEM photographs of the microcapsules syn- increase of (St + MMA) monomer weight (5.0–10.0 g). When
thesized using different amounts of the (St + MMA) monomers. the weight was increased up to 12.0 g, the thickness did not

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Fig. 6 (A) TEM photographs of the microcapsules synthesized with different amounts of (St + MMA) monomers (g): (a) 5.0; (b) 6.0; (c) 7.0; (d) 9.0;
(e) 10.0; and (f ) 12.0. The scale bars denote 5 μm. (B) Relationship of the release time of APS from the microcapsules with the polymer shell thickness
of the microcapsules. Other conditions: pH = 7.0, T = 60 °C, [NaCl] = 100 mg L−1.

obviously change (Fig. 6A(f )). As shown in Fig. 6B, as the thick-
ness increased, the beginning of the release time of APS from
the microcapsules also increasd. Therefore, Fig. 5 and 6 indi-
cate that we can control the burst release time of the micro-
capsules by adjusting the temperature, NaCl concentration
and thickness of the copolymer shell.
Storage stability of the microcapsules
The morphologies and dispersion of the APS microcapsules
were obtained by OM and DLS before and after they were
stored for 5 months at room temperature. As shown in Fig. 7,
the morphologies and dispersion of the microcapsules were
almost the same for both samples.32 The only slight difference

Fig. 7 OM and DLS photographs of (a, c) APS microcapsules, and (b, d) APS microcapsules stored for 5 months at room temperature. Inset in
(b) shows the controlled release profiles of the encapsulated APS of samples (a) and (b). Other conditions: 1% w/w APS microcapsules were added to
100 mL distilled water at pH 7.0 and 70 °C.

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Fig. 8 FE-SEM (a) and TEM (b) of the sodium nitrite microcapsules synthesized with the above mentioned method. (c) Controlled release behavior
of the encapsulated sodium nitrite monitored by a conductivity meter. Other conditions: 1% w/w sodium nitrite microcapsules were added to
100 mL distilled water.
was that the controlled burst release time slightly shortened
for the microcapsule samples stored for 5 months (inset of
Fig. 7b). This is because a little water was carried into the
conical flask during the process of washing the synthesized
microcapsules with distilled water, which made the microcap-
sules swell slightly when stored for 5 months.
Synthesis of microcapsules containing sodium nitrite
As shown in Fig. 8, microcapsules with sodium nitrite encap-
sulated were also available by this method. The FE-SEM photo-
graphs of the shell surface of the microcapsules (Fig. 8a) were
the same as those mentioned before (Fig. 3). The microcap-
sules were distinct core–shell structures and the diameter of
the microcapsules was 10–14 μm (Fig. 8b). We found that the
release pattern of the prepared microcapsules was also burst
release. In addition, it is worth noting that the start time of
the burst release ranged from 7 to 36 h, which is shorter than
in Fig. 5a (10–45 h). This can be explained by the fact that
some of the monomers (St–MMA) were firstly initiated by APS
to form the copolymer shell (P(St–MMA)), and then the excess
monomers were initiated by AIBN to coat the exterior surface
with the driving force caused by the evaporation of dichloro-
methane. The shell of the APS microcapsules prepared by this
method can be considered as two layers. However, the copoly-
mer shell of the sodium nitrite microcapsules was just
initiated by AIBN (one layer).
4. Conclusions
We have demonstrated a novel and facile evaporation–dis-
persion–polymerization method to synthesize microcapsules
containing water-soluble cores. With this method, water-
soluble materials can be encapsulated into the microcapsules
effectively and then subjected to controlled burst release from
the microcapsules within a given region of time. This method
is expected to be applied in catalysis, drug delivery, biotechno-
logy and many other applied fields.
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Acknowledgements
This work was supported by the National Natural Science
Foundation of China (20573091), the Project Funded by the
Priority Academic Program Development of Jiangsu Higher
Education Institutions and the Educational Committee of
Jiangsu Provincial General Universities Graduate Student
Scientific Research Invention Plan (CXLX13_898). For this
work, we thank the Testing Center of Yangzhou University for
the materials’ characterization.
References
1 Y. J. Zhao, H. C. Shum, L. L. A. Adams, B. J. Sun, C. Holtze,
Z. Z. Gu and D. A. Weitz, Langmuir, 2011, 27, 13988–13991.
2 M. Windbergs, Y. J. Zhao, J. Heyman and D. A. Weitz, J. Am.
Chem. Soc., 2013, 135, 7933–7937.
3 A. M. Pavlov, G. B. Sukhorukov and D. J. Gould, Bio-
macromolecules, 2013, 14, 608–612.
4 B. X. Liu, X. Zhou, F. Yang, H. Shen, S. G. Wang, B. Zhang,
G. Zhi and D. C. Wu, Polym. Chem., 2014, 5, 1693–1701.
5 A. C. Karaca, N. Low and M. Nickerson, J. Agric. Food
Chem., 2013, 61, 5148–5155.
6 A. A. Aydın, Chem. Eng. J., 2013, 231, 477–483.
7 J. Zhang, X. D. Xu, Y. Liu, C. W. Liu, X. H. Chen, C. Li,
R. X. Zhuo and X. Z. Zhang, Adv. Funct. Mater., 2012, 22,
1704–1710.
8 R. Shenoy, M. W. Tibbitt, K. S. Anseth and C. N. Bowman,
Chem. Mater., 2013, 25, 761–767.
9 T. Trongsatitkul and B. M. Budhlall, Langmuir, 2011, 27,
13468–13480.
10 S. Neuser and V. Michaud, Polym. Chem., 2013, 4,
4993–4999.
11 Y. K. Song and C. M. Chung, Polym. Chem., 2013, 4,
4940–4947.
12 B. Samanta, X. C. Yang, Y. Ofir, M. H. Park, D. Patra,
S. S. Agasti, O. R. Miranda, Z. H. Mo and V. M. Rotello,
Angew. Chem., Int. Ed., 2009, 48, 5341–5344.
This journal is © The Royal Society of Chemistry 2014

Polymer Chemistry
13 K. A. Bogdanowicz, B. Tylkowski and M. Giamberini,
Langmuir, 2013, 29, 1601–1608.
14 M. Windbergs, Y. J. Zhao, J. Heyman and D. A. Weitz, J. Am.
Chem. Soc., 2013, 135, 7933–7937.
15 H. Y. Chen, Y. Zhao, Y. L. Song and L. Jiang, J. Am. Chem.
Soc., 2008, 130, 7800–7801.
16 Q. M. Ji, M. Miyahara, J. P. Hill, S. Acharya, A. Vinu,
S. B. Yoon, J. S. Yu, K. Sakamoto and K. Ariga, J. Am. Chem.
Published on 30 June 2014. Downloaded by University of Illinois at Chicago on 24/10/2014 11:03:46.
Soc., 2008, 130, 2376–2377.
17 O. Shchepelina, M. O. Lisunova, I. Drachuk and
V. V. Tsukruk, Chem. Mater., 2012, 24, 1245–1254.
18 Y. J. Zhao, H. C. Shum, L. L. A. Adams, B. J. Sun, C. Holtze,
Z. Z. Gu and D. A. Weitz, Langmuir, 2011, 27, 13988–13991.
19 X. L. Wang, J. F. Shi, Z. Y. Jiang, Z. Li, W. Y. Zhang, X. K. Song,
Q. H. Ai and H. Wu, Biomacromolecules, 2013, 14, 3861–3869.
20 X. Q. Chen, F. C. Shu, W. P. Li, G. Y. Hua, X. J. Xiang and
L. C. Geng, Dril. Fluid Compl. Fluid., 2010, 27, 33–37.
21 Q. B. Tang, B. B. Wang, Y. Q. Shi, L. Song and Y. Hu, Ind.
Eng. Chem. Res., 2013, 52, 5640–5647.
22 G. B. Huang, H. C. Guo, J. G. Yang, X. Wang and J. R. Gao,
Ind. Eng. Chem. Res., 2013, 52, 4089–4097.
This journal is © The Royal Society of Chemistry 2014
View Article Online
Paper
23 X. R. He, C. Han, X. Wang, K. Li and Z. X. Nuobu,
J. Southwest Pet. Univ., 2010, 32, 130–134.
24 D. Wang, J. Y. Wang, W. T. Wang, H. Zhang, G. F. Li and
X. Y. Zhang, Oilfield Chem., 2003, 20, 220–223.
25 F. Kuang, J. Wang, F. Jia and Z. B. Ye, Corros. Sci. Prot.
Technol., 2009, 21, 173–175.
26 L. Y. Chu, S. H. Park, T. Yamaguchi and S. Nakao,
Langmuir, 2002, 18, 1856–1864.
27 F. G. Guo, Q. Y. Zhang, B. L. Zhang, H. P. Zhang and
L. Zhang, Polymer, 2009, 50, 1887–1894.
28 H. R. Liu and J. H. Du, Solid State Sci., 2006, 8, 526–
530.
29 O. Parlak and M. M. Demir, ACS Appl. Mater. Interfaces,
2011, 3, 4306–4314.
30 N. B. Shukla, S. Rattan and G. Madras, Ind. Eng. Chem. Res.,
2012, 51, 14941–14948.
31 M. Wrede, V. Ganza, J. Bucher and B. F. Straub, ACS Appl.
Mater. Interfaces, 2012, 4, 3453–3458.
32 S. Erokhina, L. Benassi, P. Bianchini, A. Diaspro,
V. Erokhin and M. P. Fontana, J. Am. Chem. Soc., 2009, 131,
9800–9804.
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