Article

pubs.acs.org/IECR

Green Preparation of Expandable Graphite and Its Application in

Flame-Resistance Polymer Elastomer
Jindu Huang,†,§ Qianqiu Tang,†,§ Weibin Liao,† Gengchao Wang,*,† Wei Wei,‡ and Chunzhong Li†
†
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Key Laboratory of Advanced Polymeric Materials, School
of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China
‡
Jiangsu Xinghua Rubber Belt Co., Ltd., Haian, Jiangsu 226600, P. R. China
*
S Supporting Information

ABSTRACT: Although research on expandable graphite (EG)

has achieved great progress, its practical application is restricted
due to high sulfur content and serious pollution during
production. Herein, low-sulfur EG was prepared through a
two-step intercalation method using environmentally friendly
hydrogen peroxide as an oxidant. By optimizing reaction
parameters and process, the as-prepared EG exhibits low sulfur
content (1.85 wt %) and high exfoliation volume (282 mL g−1).
Moreover, when 30 wt % EG is mixed with ethylene-vinyl
acetate copolymer (EVM) matrix, the obtained EG/EVM
composite exhibits a high limited oxygen index (LOI) of
30.4%, showing its excellent flame retardancy. Furthermore, for
the compatibility between EG and EVM to be improved, poly(vinyl acetate) (PVAc) was grafted to EG by in situ radical
polymerization. The EG-g-PVAc/EVM composite shows high flame resistant performance with improved control of fly ash.
Therefore, this easily prepared EG can be broadly applied in environmentally friendly polymeric flame-resistance field.

1. INTRODUCTION which refers to the sudden expansion of the expandable

Expandable graphites (EGs), including most acceptor-type
graphite intercalation compounds (aGICs) and especially
GICs-bisulfate, have been considered as an ideal flame retardant
additive in polymer matrix due to its low cost, low smoke,
antidripping melt, and halogen-free characteristics.1−8 During
abrupt thermal shock or fire, with the decomposition and
evaporation of intercalation guests of EG flakes pushing the
adjacent graphene layers apart from each other, EG flakes in the
polymer composite will expand several-hundred-fold in volume
and form wormlike exfoliated graphite to isolate material from
heat and air.9 Generally, GICs-bisulfate is synthesized by a
chemically oxidative intercalation method using strong
oxidizing agents (e.g., concentrated nitric acid, potassium
permanganate, potassium dichromate, chromium trioxide, etc.)
and concentrated sulfuric acid.10−18 The redox potential of the
above-mentioned strong oxidizing agents is high enough to
oxidize carbon atoms at plane edges and in defects,19−21
forming macrocation Cn+ for subsequent intercalation of anions
and molecules.22,23 However, these conventional oxidizing
agents bring severe pollution and hazards during the
production and use of EG.24 Moreover, these kinds of EG
release a certain amount of toxic gases like sulfur oxide16 and
nitric oxide25 in fire, polluting the environment and severely
harming human health. It is also found that heavy fly ash is
emitted during combustion of EG/polymer composites,
reducing the flame-resistance effect as a result.26,27 Further-
more, this phenomenon is also known as a “popcorn effect”,
graphite when suddenly exposed to high heat.28−30
The trend of sustainable development has set a higher
demand on environmental friendliness and safety of materials.
Various methods have been proposed to reduce or even
eliminate the sulfur content of EG. Most of these methods
adopt perchloric acid,31−34 hydrochloric acid,35 nitric acid,36−38
boric acid,39 and so forth, which may introduce new pollutants
or hazardous chemicals. Recently, the electrochemical inter-
calation method has been claimed to be environmentally
friendly as it uses dilute acid concentrations without chemical
oxidizing agents.40,41 However, the installation of the electro-
chemical reaction is complicated, and this method also features
low yield and high cost.
Herein, we report a novel mild two-step intercalation method
to prepare low-sulfur EG using environmentally friendly
hydrogen peroxide as an oxidant, avoiding the use of high-
pollution oxidizing agents such as nitric acid, potassium
dichromate, and so forth. First, natural flake graphite (NFG)
was preoxidized by hydrogen peroxide before sulfuric acid
intercalation. Second, first intercalation compounds were
preoxidized again, and then concentrated phosphoric acid was
added to replace some of the sulfate anions or sulfuric acid
Received: December 16, 2016
Revised: April 17, 2017
Accepted: April 24, 2017
Published: April 24, 2017

© XXXX American Chemical Society A DOI: 10.1021/acs.iecr.6b04860

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Industrial & Engineering Chemistry Research
molecules. Furthermore, high flame resistant thermoplastic
elastomer with improved control of fly ash was obtained by
melt blending of EG-grafted poly(vinyl acetate) together with
ethylene-vinyl acetate copolymer (EVM).
2. EXPERIMENTAL SECTION
2.1. Materials. Natural flake graphite (NFG, 300 μm, ≥99.9
wt %) was purchased from Qingdao Tianheda Graphite Co.,
Ltd., China. Hydrogen peroxide (H2O2, 30 wt %), sulfuric acid
(H2SO4, 98 wt %), and phosphoric acid (H3PO4, 85 wt %)
were received from Shanghai Lingfeng Chemical Reagent Co.,
Ltd., China. H3PO4 was concentrated (≥99.9 wt %) by mixing
with the appropriate amount of phosphorus pentoxide.38
Azobis(isobutyronitrile) (AIBN, analytical grade) was obtained
from Sinopharm Chemical Reagent Co., Ltd. and purified by
recrystallizing from a mixed solution of ethanol and deionized
water (1:1). Vinyl acetate monomer (VAc) was supplied by
Shanghai Aladdin Bio-Chen Technology Co., Ltd. Ethylene-
vinyl acetate copolymer (EVM, Levapren 500HV, 50 wt % vinyl
acetate content, 27 ± 4 cps Mooney viscosity, ≤5 g/10 min
melt flow index, 1.00 g/cm3 density) was a product of Lanxess
Chemical Co., Ltd.
2.2. Synthesis of Expandable Graphite. Initially, 3 g of
NFG was preoxidized by H2O2 (0.4−0.8 mL) for 60 min under
mechanical stirring and ultrasonication at ambient temperature.
Then, H2SO4 (8−12 mL) was added slowly to the above
mixture and stirred at various temperatures (20−60 °C) and
times (60−140 min). The resulting mixture was filtered,
washed repeatedly with deionized water and dried at 65 °C for
12 h to obtain the first intercalation compounds (EG-1).
Second preoxidation treatment was applied to 1 g EG-1 (the
same as the above preoxidization process). Subsequently, 3 mL
concentrated H3PO4 was added slowly and was stirred at
various temperature (20−60 °C) and time (20−180 min). The
resulting product was washed with deionized water, and dried,
successfully achieving expandable graphite (EG-2) with low
sulfur content.
2.3. Preparation of Expandable Graphite-Grafted
Poly(vinyl acetate). Expandable graphite-grafted poly(vinyl
acetate) (EG-g-PVAc) was prepared by in situ free radical
polymerization of VAc at edges of EG-2 (shown in Figure S1),
and the detailed procedure is as follows: First, 20 g of VAc was
dissolved in 50 mL of butyl acetate. Then, 10 g of EG-2 was
added to the solution and stirred for 30 min. Then, 0.2 g of
AIBN was added slowly to the above solution. The polymer-
ization was kept at 65 °C for 24 h under an argon atmosphere.
The resulting product was washed with butyl acetate several
times and dried at 50 °C under vacuum for further use.
2.4. Preparation of Flame-Resistant EG/EVM Compo-
sites. EVMs were blended with EG-1, EG-2, and EG-g-PVAc in
various proportions on Thermo Haake rheomixer at 100 °C for
10 min with a rotation speed of 60 rpm. The samples of the
composites were obtained by press molding at 120 °C for 8
min. The size and thickness of the samples were dependent on
different test requirements.
2.5. Characterization. The exfoliation volume (EV) was
determined by exfoliating the prepared EG particles (M1 gram)
in a quartz beaker with scale line by heating it in a muffle
furnace at 800 °C for 60 s.40 The volume (V) of exfoliated
product was recorded, and the mass (M2) was obtained by
analysis balance. The EV and weight loss rate (WL) were
calculated by following formulas: EV = V/M1, WL = (M1 −
M2)/M2
B DOI: 10.1021/acs.iecr.6b04860
Article
X-ray diffraction (XRD) data were collected by a Rigaku D/
Max 2550 VB/PC X-ray diffractometer using Cu Kα radiation
with the 2θ angle from 10−50°. Raman spectra were obtained
with an inVia Reflex Raman spectrometer using a 50 mW He−
Ne laser at 514 nm. X-ray photoelectron spectroscopy (XPS)
analysis was performed on an ESCALAB 250Xi X-ray
photoelectron spectrometer equipped with a monochromatic
Al Kα X-ray source. The morphologies of the samples were
observed by scanning electron microscopy (SEM, Hitachi
S3400) and field-emission scanning electron microscopy (FE-
SEM, Hitachi S4800). The elemental study of raw and
intercalated graphite was investigated using a Vario EL Cube
elemental analyzer. The Fourier transform infrared spectrosco-
py (FTIR) spectra were characterized using a Nicolet 6700
spectrometer equipped with a Smart OMIN Sampler.
The limited oxygen index (LOI) of the composites was
performed on a JF-3B oxygen index tester according to ASTM
D2863 with the size of all samples to be 150 × 6 × 3 mm3.
Cone calorimeter tests were carried out with an FTT cone
calorimeter according to ISO 5660. All samples, of dimensions
100 × 100 × 3 mm3, were wrapped in aluminum foil and
exposed horizontally to an external heat flux of 35 kW m2. For
each formulation, the test was repeated three times, and the
experimental error was ±5%. The mechanical properties of the
composites were measured on a CMT 2203 testing system
according to ASTM D638.
3. RESULTS AND DISCUSSION
3.1. Optimization of Preparation Conditions. High
exfoliation volume (EV) of expandable graphite is the key for
improving the level of flame retardancy.42 For high-perform-
ance expandable graphite to be obtained, the preparation
parameters and conditions of EG-1 were optimized by
orthogonal method.32 According to standard 34 orthogonal
experimental design, the factors (temperature and time of
H2SO4 intercalation, dosage of H2SO4 and H2O2) and levels are
listed in Table S1, which can be arranged into nine reactions
(Table S2). The treatment results are shown in Figure 1. The
height of the column represents the average value of EV of
three products in each level under one factor. The bigger range
indicates the greater influence of the factor to EV. By the
calculations, the ranges of four factors (temperature, time, and
dosage of H2SO4 and H2O2) are 40, 26, 9, and 8, respectively.
Obviously, the value of EV is contributed mainly by
Figure 1. Column graph of orthogonal design results of EG-1. The
levels of each factor are as follows: 30, 40, and 50 °C for temperature;
40, 60, and 80 min for intercalation time; 8, 10, and 12 mL for dosage
of H2SO4, and 0.4, 0.6, and 0.8 mL for dosage of H2O2.
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Figure 2. Exfoliation volume and weight loss as functions of the temperature and intercalation time for expandable graphite by (a, b) first and (c, d)
second step intercalation.

Figure 3. (a) XRD patterns and (b) Raman spectra of natural flake graphite (NFG), EG-1, and EG-2.

temperature and time in the process of intercalation. However,
dosage of H2O2 and H2SO4 have limited effects on EV.
On the basis of these data, further studies have been carried
out with single factor (temperature: 20−60 °C; time: 60−140
min) experiments under certain dosages of H2SO4 (10 mL) and
H2O2 (0.8 mL) (Figure 2a and b). The optimum conditions
(80 min, 40 °C) are obtained, and the maximum EV is up to
240 mL g−1. Moreover, it can be seen that the weight loss (WL)
is positively correlated with EV in first step intercalation, which
is because, during the exfoliation process of EG, gases are
released resulting from the volatilization and decomposition of
hydrogen sulfate anions and sulfuric acid molecules and the
released gases make the volume of EG larger at the same time.
In the temperature range of 40−60 °C and intercalation time
range of 80−140 min, overoxidation occurs following
deintercalation of inserts; thus, EV decreases. Furthermore,
compared with intercalation temperature, EV does not change
much with longer intercalation time. Thus, it can be said that
EV is more sensitive to temperature, which is due to the fact
that there is a higher tendency for volatilization of intercalates
and decomposition of H2O2 under high temperature, further
confirming the results of the orthogonal experiment.
C DOI: 10.1021/acs.iecr.6b04860
Similarly, synthesis conditions of EG-2 have been optimized
by using optimal EG-1 as raw material as shown in Figure 2c
and d. It is interesting that EG-2 obtains considerably higher
EV (up to 282 mL g−1) than that of EG-1 under the interaction
temperature of 40 °C and time of 100 min. It is noteworthy
that, different from EG-1, the WL and EV of EG-2 seem
negatively correlated in the temperature range of 20−40 °C and
intercalation time range of 20−100 min, which will be studied
below.
3.2. Structure and Morphology Characterization of
EG-1 and EG-2. XRD and Raman analysis were conducted to
investigate the oxidation and intercalation effects of EG-1 and
EG-2. For the untreated graphite, the sharp peak at 26.6°
corresponds to the 002 crystal phase of pure graphite (Figure
3a). In comparison, EG-1 and EG-2 exhibit broader dominant
diffraction peaks at lower angle (2θ = 26.0°), which is due to
the expansion of c-axis of graphite and the increasing lattice
defects such as stacking disorder43 resulting from the addition
of oxygen-containing functional groups and intercalation of
anions and molecules into the graphite. The disordered
structure can be verified by the Raman spectra as well (Figure
3b). As we known, the D-band is associated with disorder-
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induced scattering resulting from imperfections or loss of
hexagonal symmetry of disordered graphite. The G-band
corresponds to an E2g mode of graphite and is related to
vibration of sp2-bonded carbon atoms in a two-dimensional
hexagonal lattice.44 Therefore, the peak intensity ratio of D-
and G-bands (ID/IG) was applied to evaluate the regularity of
the graphite structure.45 As calculated, the ID/IG ratios of NFG,
EG-1, and EG-2 are 0.076, 0.115, and 0.279, respectively, which
suggests that the graphitic crystalline structure has been further
damaged with increasing defect by two-step intercalation.
Furthermore, the SEM images (Figure 4) of exfoliated EG-1
and EG-2 show an expanded wormlike structure. For
Figure 4. SEM images of (a, b) exfoliated EG-1 and (c, d) exfoliated
EG-2 at magnifications of 300× and 1000×.
comparison, NFG and its high temperature treatment product
exhibit a densely packed lamellar structure (shown in Figure
S2). It suggests that only a sudden heating process will not lead
to the expansion of graphite. Instead, the wormlike structure of
EG comes from decomposition of intercalated sulfur
compounds under high temperature. Moreover, compared
with exfoliated EG-1 (Figure 4a and b), exfoliated EG-2 (Figure
4c and d) obtains more and tighter cellular structure, which
verifies its increase of inserted layers and deintercalation of
sulfur compounds. For the change in sulfur content of EG-2 at
different intercalation times and temperatures to be confirmed,
elemental analysis results (Figure S3) were obtained using an
element analyzer. The results show that the sulfur content
decreases with increasing intercalation time and temperature;
thus, the WL will decrease correspondingly, which reasonably
explains the negative correlation between WL and EV of EG-2.
3.3. Chemical Composition Analysis of EG-1 and EG-2.
For the intercalated element content of EG-1 and EG-2 to be
further quantified, XPS and Element Analysis were adopted.
The XPS spectra of EG-1 (Figure 5c) and EG-2 (Figure 5e)
show obviously stronger O 1s peaks (∼532 eV) than that of
NFG (Figure 5a), indicating the introduction of a large amount
of oxyacid. In the case of EG-2, after two-step oxidative
intercalation, appearance of a P 2p peak (∼135 eV) and
weakening of the S 2p peak (∼169 eV) were observed from the
enlarged views, showing the introduction of a P element and
decrease in the content of the S element for EG-2.
Furthermore, the element analysis also shows that the sulfur
content of EG-2 (1.85 wt %) is lower than that of EG-1 (3.74
wt %) as shown in Table 1.
D DOI: 10.1021/acs.iecr.6b04860
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Moreover, the overlapping C 1s peaks of both were resolved
by curve fitting (Figure 5b, d, and f). The peak area at 286.2 eV
(green peak) is related to the amount of oxidized carbon (i.e.,
C−OH, C−O−C, and CO bonds) at the edge of the
sheets.10,45 It can be calculated that the peak area ratio of the
oxidized carbon to conjugated CC bond structure (284.5 eV,
blue peak) for EG-2 is 11.6%, which is more than that of EG-1
(8.2%) and nearly twice that of NFG (6.3%). Thus, the XPS
results further demonstrate the process of twice oxidation.
3.4. Formation Mechanism of Expandable Graphite.
For the process of two-step oxidative intercalation to be
determined, a scheme of exchange-and-diffusion intercalation
was proposed. As shown in Figure 6, after the second
preoxidation for EG-1, more original graphite galleries are
enlarged resulting from the addition of oxygen-containing
functional groups at plane edges and defects. Moreover, during
the second intercalation process, exchange between sulfur
compounds and phosphoric compounds occurs due to a
concentration difference effect. Furthermore, the mixture acid
solution diffuses into new graphite grids and remains stable.
After being washed and dried, EG-2 with low sulfur content was
prepared. From the section morphologies of EG-1 and EG-2, it
is obvious that EG-2 owns more detached sheets than that of
EG-1. This macroscopic delamination damage may have been
caused by large-scale oxidation, which indicates further
disordering of graphite, leading to more insertion.
3.5. Flame-Resistant and Mechanical Properties of
Composites. The flammability properties of flame-resistant
EG-1/EVM and EG-2/EVM composites were analyzed by
limited oxygen index (LOI). From Figure 7, it can be seen that,
with the increase of EG content, the LOI values of EG-1/EVM
and EG-2/EVM increase from 23.1 to 29.5% and 23.3 to 30.4%,
respectively, which suggests that EG-2 enhances flame
resistance for EVM. The reason for the improvement can be
explained as follows. On the one hand, phosphorus guests
between graphite layers of EG-2 will carbonize the polymeric
matrix rapidly in fire because of its strong dehydration property.
On the other hand, the char layers from polymer carbonization
form strong adhesion with wormlike exfoliated graphite, which
prevents the underlying material from heat and mass transfer
with the outside fire. Thus, the flame retardancy of EG-2/EVM
will be improved.
However, because of the weak cohesiveness between
inorganic graphite and organic polymeric matrix, rich fly ash
will rise sharply during combustion, limiting the application of
EG. Furthermore, the addition of EG may sharply deteriorate
the mechanical properties of matrix resin materials because of
their poor compatibility.46,47 Therefore, we attempt to graft
organic poly(vinyl acetate) (PVAc) to EG-2 by in situ free
radical polymerization to improve its compatibility and
cohesiveness with EVM matrix. From the FTIR spectra of
EG-2 and EG-g-PVAc in Figure S4, the characteristic peaks at
1228 and 1733 cm−1 correspond to the C−O and CO in the
ester group of PVAc. Even FTIR cannot prove the successful
grafting, it is thought that the grafting is the objective and it is
likely that it happened.
It can be seen from the FE-SEM images of EG-2/EVM
(Figure 8a) that EG particles are curly and distinct in matrix,
and there is a huge gap (Figure 8b, marked with a red arrow) in
the phase interfaces, indicating incompatibility between EG
particles and EVM matrix. In comparison, EG-g-PVAc in EVM
(Figure 8c) becomes smooth and homogeneous and exhibits
tight cohesiveness (Figure 8d, marked with blue arrows) with
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Figure 5. XPS spectra with survey scan (a) NFG, (c) EG-1, and (e) EG-2 and C 1s core level XPS spectra for (b) NFG, (d) EG-1, and (f) EG-2.

Table 1. Element Analysis of NFG, EG-1, and EG-2 EVM continuous phase without an obvious interface. This is
because the existence of PVAc functions as a bridge between
sample C (wt %) S (wt %)
the inorganic part of EG and organic part of EVM.
NFG 97.8 nil
Because of its chemical structure and homogeneous
EG-1 74.2 3.74
EG-2 76.2 1.85
morphology, EG-g-PVAc is an ideal candidate for flame-
resistant materials, especially thermoplastic elastomers. The
digital photo shows that the ignition of EG-g-PVAc/EVM

Figure 6. Schematic illustration of the green preparation process of expandable graphite.

E DOI: 10.1021/acs.iecr.6b04860
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Figure 7. LOI as a function of EG content for EG-1/EVM and EG-2/
EVM composites.
(Figure 9c) was more stable with lower smoke and less fly ash
compared with that of EG-2/EVM (Figure 9a). The residual
expanded char layers of EG-2/EVM (Figure 9b) were fluffy and
easily flake away from the substrate. In contrast, the carbon
residues of EG-g-PVAc/EVM (Figure 9d) were compact and
adhesive on the surface. The LOI of EG-g-PVAc/EVM is 28.7%
compared to 27.9% of EG-2/EVM when the filler is 20 wt % in
both composites (shown in Table S3), showing the enhanced
flame resistance of EG via the grafting process. In addition,
mechanical performances were measured by tensile testing. The
stress−strain curves (Figure S5) show that the EG-g-PVAc/
EVM composite acquires better mechanical properties than
those of EG-2/EVM. This may be due to the fact that the huge
gaps between large EG particles and EVM may function as
stress defect points during the stretching process, leading to
sharply reduced tensile strength and breaking elongation. In
comparison, surface modification of EG by PVAc narrows or
even eliminates the gap, thus delaying the occurance of
breakage.
Figure 8. FE-SEM images of the low temperature brittle fracture face of (a, b) EG-2/EVM and (c, d) EG-g-PVAc/EVM at magnifications of 100×
and 1000×.
F DOI: 10.1021/acs.iecr.6b04860
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Figure 9. Digital photos of ignition and residue of (a, b) EG-2/EVM
and (c, d) EG-g-PVAc/EVM.
The cone calorimeter test, an effective bench-scale apparatus
to simulate real fire scenarios, has been widely used to evaluate
the flammability characteristics of polymeric materials.48 The
curves of heat release rate (HRR) and total smoke release
(TSR) curves at a heat flux of 35 kW m−2 are given in Figure
10. The related time to ignition (TTI), peak HRR (PHRR),
total heat release (THR), and average specific extinction area
(SEA) are also recorded in Table 2. The TTI of EG-g-PVAc/
EVM decreased to 33 from 46 s of pure EVM, which may be
due to the high thermal conductivity of EG.49 However, the
flame-resistant EG-g-PVAc/EVM composite showed a dramatic
decline of the HRR and TSR curves with prolongation of the
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Figure 10. (a) Heat release rate (HRR) and (b) total smoke release (TSR) curves of pure EVM and flame-resistant EG-g-PVAc/EVM composite.

Table 2. Cone Test Results of Pure EVM and Flame- flame-resistant and mechanical properties of EVM, EG-
Resistant EG-g-PVAc/EVM Composite 2/EVM, and EG-g-PVAc/EVM (PDF)

sample
TTI
(s)
PHRR
(kW m−2)
THR
(MJ m−2)
TSR
(m2 m−2)
average
SEA
(m2 kg−1) FPI
■ AUTHOR INFORMATION
Corresponding Author
EVM 46 790.8 107.8 1958.0 518.9 0.058 *Tel.: +86 21 64253527. E-mail: gengchaow@ecust.edu.cn.
EG-g- 33 124.5 68.8 107.2 33.7 0.265
PVAc/ ORCID
EVM Gengchao Wang: 0000-0002-5421-0164
Author Contributions
§
J.H. and Q.T. contributed equally to this work.
combustion time, and the PHRR and TSR values were reduced Notes
by 84.3 and 94.5%, respectively. In addition, the increased fire The authors declare no competing financial interest.
performance index (FPI, defined as the proportion of TTI and
PHRR) of EG-g-PVAc/EVM suggests its great safety in a fire
hazard. The modified EG may tend to form compact and
■ ACKNOWLEDGMENTS
We greatly appreciate the financial support of the National
continuous graphite worms in fire, which can act as a physical Natural Science Foundation of China (51673064), Shanghai
barrier to prevent heat transfer from heat source and smoke Municipality Research Project (15520720500), and the Special
from substrate.42,50 As a result, the flame retardancy of EVM Fund of Jiangsu Province for Scientific and Technological
with EG-g-PVAc is significantly enhanced, which is also Achievements Transformation (BA2016119).
confirmed by the decrease of THR and average SEA.

4. CONCLUSIONS
In this paper, a simple two-step intercalation method to prepare
EG has been put forward. With conditions optimized, the
prepared product obtains high exfoliation volume (282 mL g−1)
and low sulfur content (1.85 wt %) with a certain amount of
phosphorus between graphite layers. Analysis of the morphol-
ogy, structure, and elements has validated the two-step
exchange-and-diffusion intercalation process. LOI of the EG-
2/EVM composite can reach 30.4% when the filler content is
30 wt %. By grafting PVAc via in situ radical polymerization,
EG had stronger interfacial adhesion with polymer matrix; the
EG-g-PVAc/EVM composite exhibits enhanced flame retard-
ancy and mechanical properties, and the fly ash has been
effectively controlled during combustion. In summary, this
investigation provides an easy and environmentally friendly
preparation method for modified low-sulfur expandable graph-
ite, which can be broadly applied in green polymeric fire
resistance in the foreseeable future.
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■
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
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Schematic diagram of EG-g-PVAc, orthogonal table of
samples, micromorphology of NFG and its high
temperature treatment product, sulfur content of EG-2
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