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Enhanced Thermal and Mechanical Properties of Polyimide/Graphene Composites Wen Dai, Jinhong Yu*, Yi Wang, Yingze Song, Hua Bai, Kazuhito Nishimura, Huiwei Liao*, and Nan Jiang* Macromol. Res., 22, (2014) The incorporation of graphene sheets increased the thermal conductivity, thermal sta- bility and mechanical properties of polyimide matrix.

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Enhanced Thermal and Mechanical Properties of Polyimide/GrapheneComposites

Wen Dai, Jinhong Yu*, Yi Wang,Yingze Song, Hua Bai, Kazuhito Nishimura,Huiwei Liao*, and Nan Jiang*

Macromol. Res., 22, (2014)

The incorporation of graphene sheets increased the thermal conductivity, thermal sta-bility and mechanical properties of polyimide matrix.

Page 2: Enhanced Thermal and Mechanical The incorporation of ...marinelab.nimte.cas.cn/archives/201312/W020140725471395796437.pdf · Enhanced Thermal and Mechanical Properties of Polyimide/Graphene

Macromolecular Research

The Polymer Society of Korea

www.springer.com/13233

pISSN 1598-5032 eISSN 2092-7673

Enhanced Thermal and Mechanical Properties of Polyimide/Graphene

Composites

Wen Dai1,2, Jinhong Yu*,2,3, Yi Wang2, Yingze Song2, Hua Bai2, Kazuhito Nishimura2,

Huiwei Liao*,1, and Nan Jiang*,2

1School of Materials Science and Engineering, Southwest University of Science and Technology,

Mianyang, 621010, P.R. China2Key Laboratory of Marine New Materials and Related Technology, Zhejiang Key Laboratory of Marine

Materials and Protection Technology, Ningbo Institute of Material Technology & Engineering,

Chinese Academy of Sciences, Ningbo, 315201, P.R. China3Key Laboratory of New Processing Technology for Nonferrous Metals and Materials, Ministry of Education,

School of Material Science and Engineering, Guilin University of Technology, Guilin 541004, China

Received January 20, 2014; Revised April 7, 2014; Accepted June 6, 2014

Abstract: Polyimide (PI)/graphene sheets (GSs) composites were prepared by solution blending. The incorporation

of GSs increased the thermal conductivity, thermal stability and mechanical properties of PI. The thermal conductivity

of PI/GSs composites was significantly improved compared with that of neat PI from 0.254 W/mK to 1.002 W/mK

attribute to the homogeneous dispersion of graphene and the formation of heat conduction pathway. Furthermore,

the Young modulus of PI/GSs was raised up to 4.04 GPa, approximately a two-fold enhancement in comparison with

that of neat PI. In addition, the incorportation of GSs in PI indicated excellent optical transparency at the lowest

weight fractions of GSs and modified wettability of PI films.

Keywords: polyimide, graphene, composites, thermal properties, mechanical properties.

Introduction

Aromatic polyimides (PI) are widely used in microelec-

tronics and aerospace industries as a material for electronic

packaging and electrical insulating due to their superior

mechanical properties, high thermal and chemical stabilities

and low dielectric constant.1-4 However, the PI polymers are

thermally insulating and have a thermal conductivity of only

about 0.2 W/mK,5 which cannot meet the heat-dissipating

requirements of modern electronic and electrical systems.

Therefore, improvement of the thermal conductivity of polymer

becomes important. In recent years, what has been paid much

attention is that various of fillers including alumina (Al2O3),6 alu-

minum nitride (AlN),7 boron nitride (BN),8 carbon nanotube

(CNT)9 and graphene sheets (GSs),10 with high intrinsic thermal

conductivity, are used as filler to strengthen the thermal conductiv-

ity of polyimides. Among these fillers, graphene have received

great attention due to their exceptional thermal, mechanical

and electrical properties.11-14

Graphene is a monatomic thick quasi two dimensional

nanostructure consisting of sp2 hybridized six membered carbon

rings with micrometer sized horizontal dimension.15 Prossessing

extremely high aspect ratio and high thermal conductivity

(5300 W/mK),16 graphene is considered to be the most potential

filler to enhance the thermal conductivity of polymer com-

posites. However, it is difficult to obtain composites with

excellent thermal properties and mechanical due to the poor

dispersion and weak interfacial interactions of the polymer/

GSs.4,11,17 Though much work have focused on how to improve

the thermal and mechanical properties of the composites by

changing the interface properties of the composites,18,19 it is

still one of the hardest challenges in polymer composite design

to achieve the desired performance.

Hence, we report a rapid and simple method to prepare

polymer/GSs composites with excellent thermal and mechanical

properties. The GSs is mixed with polyamic acid by using

speedmixer (DAC 150.1 FVZ-K FlackTek, Inc., Germany),

which is a machine applicable to mix viscous liquid. High-

speed blend coul achieve good dispersion. To the best of our

knowledge, it is the first time to report to prepare polyimide/

GSs composite by using speedmixer. In this paper, uniform

polyimide-based composite composites containing GSs were

successfully synthesized by the speedmixer. Meanwhile, we

focus on the examination of the relationship between structure

and properties of the polyimide/GSs composites. In particu-

DOI 10.1007/s13233-014-

*Corresponding Author. E-mail: yujinhong@nimte or

[email protected] or [email protected]

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W. Dai et al.

Macromol. Res.

lar, we correlate the role of GSs leading to the thermal and

mechanical properties of the polyimide matrix, the mor-

phology and macroscopic response of the composites with

respect to their tensile properites, thermal conductivity, ther-

mal stability, transparency and wettability properties.

Experimental

Materials. Commercial graphene sheets (GSs) were produced

by Ningbo Institute of Materials Technology and Engineering

(Zhejiang, China). Poly(amic acid) (PAA) synthesized by pyro-

mellitic dianhydride (PMDA) and 4,4-oxidianiline (ODA) were

purchased from Ningbo Cen electrical material co., Ltd

(Zhejiang, China). N,N′-dimethlylacetamide (DMAc) were

purchased Sinopharm Chemical Reagent co., Ltd, China.

Praparation of GSs/Polyimide Composites by Speedmixer.

A solution method was adopted to prepare the PI/GSs com-

posites. Firstly, GSs powder was dissolved in DMAc (1 mg/mL)

and dispersed by applying the ultrasonic wave for 48 h at

room temperature. At the same time, poly(amic acid) (PAA)

was dissolved in DMAc at room temperature. Then, the GSs

was added to a solution of PAA/DMAc, and the resulting

mixture was put into speedmixer to stirred for 4 min at 3200

rpm to obtain homodisperse mixture. The SpeedMixer is the

ideal laboratory-sized instrument for the rapid mixing and

deaeration of a wide range of materials. It quickly and effi-

ciently creates highly uniform mixtures with repeatable results.

Then the prepared mixture was casted on a clean glass sub-

strate followed by thermally imidization in a vacuum oven

at 80 oC for 2 h and 120 oC, 150 oC, 200 oC, 250 oC, 300 oC

for 1 h, respectively. The experiment details of the process

of PI/GSs composites are shown in Scheme I. Eight sets of

films were prepared with 0, 0.1, 0.5, 1.0, 2.0, 4.0, 7.0, and

11.0 wt% of GSs loading and were named as PI, PI-0.1, PI-0.5,

PI-1.0, PI-2.0, PI-4.0, and PI-11.0, respectively.

Characterization. X-ray photoelectron spectroscopy (XPS)

was carried out with a Kratos AXIS ULTR DLD spectrome-

ter, using Al Kα excitation radiation (hv=1253.6 eV). Fourier-

transform infrared (FTIR) was carried out with a NICOLET

6700 (Thermal scientific Inc. USA) instrument over the range

of 4000-400 cm-1. The Raman spectra was recorded using a

Reflex Raman System (RENISHAW plc, Wotton-under-Edge,

UK) employing a laser wavelength of 532 nm. Atomic force

microscope (AFM) measurement was conducted on a Mul-

timode SPM from Digital Instruments with NanoscopeIa

controller. The fracture surfaces of the samples were inves-

tigated using field emission scanning electron microscopy

(FE-SEM, QUANTA FEG250, USA) at an accelerating voltage

of 20 kV, and the fracture surfaces were previously coated with

a conductive layer of gold. Thermal conductivities of the

composites were measured with LFA 457 Nanoflash (NETZSCH,

Germany) according to ASTM E1461, using the measured

heat capacity and thermal diffusivity, with separately entered den-

sity data. Samples were prepared in square shape of 10.0×10.0

mm and 0.1 mm in thickness. Thermogravimetric analyses

(TGA) were performed with a TA 50 (TA Instruments, USA)

under air gas flow at a heating rate of 3 oC/min from room

temperature to 800 oC. The tensile strength was examined on

an electron omnipotence tester of universal testing machine

(UTM, 5567A, Instron, USA). The five samples in each group

with lengths of 10 cm and widths of 10 mm were prepared

with the speed of the crosshead was 1 mm/min according to

National Standard of China (GB1040-92). Ultraviolet-visible

absorption (UV-Vis) spectra were measured by a Perkin Elmer

Lambda 750S spectrometer. Sessile drop contact-angle mea-

surements were taken at room temperature with an OCA 20 opti-

cal contact-angle instrument (Dataphysics GmbH, Filderstadt,

Germany).

Result and Discussion

Characterization of GSs. The morphology of GSs was

investigated by SEM, TEM, and AFM analysis as shown in

Figure 1. Figure 1(a) shows that the SEM image exhibited

visual appearance of GSs, displaying a variety of different

size of it. The TEM and selected area electrical diffraction

(SAED) patterns of GSs revealed the at least two-layer structure

of GSs, and between each layer structure are independent of

each other, from the analysis of the two sets of diffraction

spots emerged in SAED pattern, as shown in Figure 1(b).

The morphology and thickness of GSs were further charac-

terized by AFM and the micrographs were shown in Figure

1(c). It can be clearly seen that GSs are well exfoliated, cor-

responding to a particle size range from 0.1-4 μm and the

average thickness around 1 nm. The thickness of GSs was higher

than theoretical value (0.34 nm), which was corresponded to

the multilayered structure of GSs from TEM analysis. Although

there is no unambiguous model describing the precise chemical

structure of GSs, it is known that the basal planes of GSs areScheme I. Preparation process of the PI/GSs composites.

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Macromol. Res.

decorated with epoxide and hydroxyl groups, in addition to

carbonyl and carboxyl groups. These oxygen functionalities

will alter the van der Waals interactions between the layers

and make them hydrophilic, thus facilitating their exfoliation in

aqueous media and polar solvents.20 The length (L) of 178

pieces GSs were measured by analysing AFM images. The length

data is presented as a histogram in Figure 1(d). The GSs lengths

range from 100 nm to 4 µm with a mean of <L>=1.91 µm.

Raman spectroscopy is a efficient tool to characterize car-

bon-based materials to understand the behavior of electrons

and phonons in graphene.21 Figure 2(a) shows the Raman

spectroscopy of GSs which exhibits a weak band, the D-band

nearby 1350 cm-1 arising from a defect in the carbon struc-

ture,22,23 and two strong bands: the G-band at around 1580 cm-1

that was attribute to the first order scattering of the E2g phonon

of sp2 carbon, the 2D-band at around 2750 cm-1. Therefore

the intensity ratio from the D-band to the G-band (ID/IG) provides

standard to measure disordered degree of graphene,24 which

is corresponded to the proportion of sp3-hybirdized carbon

atoms in sp2 conjugated carbon structures. The value of ID/

IG (only 0.08) demonstrates there is litter defect of this GSs

and it possess a high intrinsic thermal conductivity. 2D-band

originate from two phonon participating in resonance Raman

processes with contrary momentum.25 The researchers found

that the intensity ratio from the 2D-band to the G-band (I2D/

IG) associated with the layer of GSs. If I2D/IG>2, the graphene is

monolayer.26 The smaller the value of I2D/IG, the more lay-

ers. In this investigation, I2D/IG=0.57. It revealed the multi-

layered structure of GSs agree with the above TEM analysis.

The FTIR spectrogram were used to investigate the GSs.

From Figure 2(b), the adsorption bands appeard at 1728 cm-1

and 1651 cm-1 can be assigned to the C=O stretching vibration

of carboxyl and C=C stretching vibration of aromatic ring.

In addition, the peak at 1080 cm-1 and 1380 cm-1 are attributed

to the stretching vibrations of C-O and C-OH,31 respectively.

Furthermore, the broad band from 3400 to 3500 cm-1 can be

originated -OH stretching vibration of hydroxyl groups. The

results shows that the GSs possess some oxygen-containing

functional group. In order to further understand the atomic

percentages and the group distribution, the GSs was ana-

lyzed by X-ray photoelectron spectroscopy (XPS). The XPS

survey spectra of GSs was showed in Figure 2(c), which

exhibited three peaks assigned to C1s (95.77%), O1s (2.56%)

and N1s (1.67%). The deconvolution of the C1s peaks was

shown in the Figure 2(d). It revealed peaks at 284.58,

284.99, 286.28, 287.10, and 287.80 eV correspond to C=C10

(61.32%), C-C10 (26.77%), C-O-H32 (10.29%), C-O-C (0.16%),

and C=O(1.46%), respectively. The percentage of conjugated

carbon ring structure containing C=C and C-C is 88.09%.

The FTIR spectra of neat PI in different temperature were

investigated to monitor the imidization process. As shown

in Figure 3, the decrease of characteristic peaks in the PAA

spectra including -NH2 at 1650 cm-1 and N-H or O-H in the

range 2500-3500 cm-1 is observed with a rise of temperature.

Simultaneously, the intensities of characteristic imide peak

at 725 cm-1 (cyclic C=O bending), 1380 cm-1 (C-N stretching),

1720 cm-1 and 1780 cm-1 (symmetric and asymmetric C=O

stretching) enhance with increasing temperature. The char-

acteristic imide peak at 1380 cm-1 (C-N stretching) was chosen

to estimate the degree of imidization at different tempera-

tures of PAA. The intensity of an internal standard at 1500 cm-1

(C=C stretching in benzene ring) was selected to eliminate

the effect of test condition. The ratio of intensity at 1380 cm-1 to

that at 1500 cm-1 was calculated at various temperatures. It

was observed that rate at 300 oC and 350 oC almost equally.

This is a direct evidence to prove the fully curing of PI.

The Morphology of PI Composites. In order to understand

the relationship between structure and properties of neat PI

and PI composites, the fracture microstructure of neat PI and PI

Figure 1. (a) SEM, (b) TEM, and (c) AFM images of GSs, (d)

histograms of measured values for 178 nanosheets length.

Figure 2. The Raman spectra (a), FTIR spectra (b) and (c,d) XPS

for the GSs.

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Macromol. Res.

composites was observed by SEM, as shown in Figure 4.

The Figure 4(a) exhibit that the fracture surface of neat PI is

quite smooth with only a few dots in it, which may be attributed to

not be elastically relapsed to smooth plane after stretching

out upon mechanical deformation. The morphology and dis-

persion of GSs in PI matrix was evaluated by SEM, as shown

in Figure 4(b-h). Compared to the neat PI, the fracture surfaces of

PI composites is rough and ridged, owing to the two dimensional

geometry of GSs sheets. It is clear that the GSs were present

in the PI composites as multi-layered platelets. According to

Figure 4(b-h), the GSs platelets are isolated by PI matrix at

a lower concentration (less than 1 wt%) ,interconnected with

each other at a middle concentration (2-4 wt%) and a higher

concentration (more than 7 wt%). In addition, the GSs are curved

or even interwoven in the PI matrix, indicating that the GSs

are extremely flexible. It was obvious noted from Figure

3((b)-(d)) that the PI with a low GSs loading (less than 1 wt%)

form sea-island structure, and the PI is continuous phase.

Under this kind of structure, the fracture surface was ductile

fracture and some GSs appeared in the root of the fracture.

Figure 4((e),(f)) show less bare polyimide and the fracture

surface is more like brittle fracture with the increase of GSs

loading result in the continuity of PI broken gradually. It can

be also seen from Figure 4((g)-(h)) that the GSs platelets are

dispersed well even in PI-11.0 and some large platelet agglomer-

ates are observed. Meanwhile, it is hard to see polyimide

matrix in cross section because the GSs become a continuous

phase forming cross-linked network. The good dispersion of

GSs platelets in PI matrix should be attributed to the functional

groups on the reduced GSs, which could enhance the inter-

action between GSs and PI matrix. The oxygen functionalities

could form hydrogen bonding between the hydrogen atom

in GSs with nitrogen atoms in PI matrix, and also between

the oxygen atoms in GSs with hydrogen atom in PI matrix,

thus facilitating their dispersion in the composites. Especially, it

is worth noting that highest GSs loading (11 wt%) in Figure 4(h)

show more GSs origenting along with film surface direction

because of stereo-hindrance effect.

Thermal properties of PI Composites. The experimen-

tally determined thermal conductivities, displayed as a func-

tion of weight fraction are shown in Figure 5. It can be seen

that the addition of GSs is very effective in increasing thermal

conductivity of PI matrix. A significant enhanced thermal

conductivity is observed at high GS loading levels. When

the concentration of GSs reaches 11.0 wt% the thermal con-

ductivity of the composite sample achieves 1.002 W/mK,

which is about 4 times increase when compared with the

neat PI (0.254 W/mK) attribute to the homogeneous disper-

sion of graphene and the formation of heat conduction path-

way. It is known that phonons are responsible for thermal

conduction in amorphous polymers,27,28 The free path of phonon

Figure 3. FTIR spectra of neat PI in different temperature.

Figure 4. SEM micrographs of fractured surface of (a) PI-0, (b)

PI-0.1, (c) PI-0.5, (d) PI-1.0, (e) PI-2.0, (f) PI-4.0, (g) PI-7.0, and

(h) PI-11.0.

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Macromol. Res.

of polymer is tiny result in a lower thermal diffusivity due to

the amorphous structure of the polymer materials. Figure 5

shows that the PI-0.1 could improve thermal diffusivity by

47.6% in comparison with the neat PI. The improvement of

thermal conductivity may GSs acted as the nucleus of PAA

crystallization lead to improve the crystallization degree of

PI. The enhancement of the crystallization degree increased

the phonon free path result in enhancing the thermal diffu-

sivity. As known the factors which have influences on the

thermal conductivity of the composite are very complicated.

The contributions of the thermal conductivity enhancement

of a composite include the thermal conductivity of materials

in the composite and the interaction between them. GSs filled

in continuous PI matrix could not form a covalent bond lead

to phonon scattering serious. Thus, the interface thermal resis-

tance of composites increase with the increase of contact

area between GSs and PI. The enhancement ratios of the

thermal conductivity of the composite are much higher than

the value predicted by the Maxwell-Eucken model,29,30 which

may be attributed to the extremely high intrinsic thermal

conductivity of GSs.

Thermal Stability of PI Composites. As a sort of high-

performance engineering plastics, thermal stability is one

important property for PI-based nanocomposites. As reported

in other literature, the thermal stability of PIs are usually

improved by incorporating into inorganic filler.33 Figure 6

illustrates the typical TGA curves of PI and PI composites.

It is noted that the thermal stability (Td-10%, the 10% decom-

position temperature) of PI was only improved slightly up to

4.0 wt% GSs loading and then decreased with the increase of

GSs content. The hydroxyl grafted the GSs may act as cata-

lyst or inducement to promote PI decomposition which was

a predominant in a high GSs loading. For neat PI, the Td-10% is

541.3 oC. The maximum Td-10% value achieved 548.2 oC

with the incorporation of 4.0 wt% GSs loading, correspond-

ing to the increases by 6.9 oC. This result can be ascribed

the following reason: (1) efficient thermal capacity of the

GSs, (2) the wrinkle structure of GSs which may inset the

polymer matrix restricting the relaxation of segments, (3) the

carbon surface of GSs in the PI might play the role of a rad-

ical scavenger to delay the thermal degradation temperature

and result in improving thermal stability of PI.34,35 However,

the Td-10% value of PI-11.0 decrease to 539.5 oC due to the

heavy agglomeration of GSs in PI matrix, which can not

affect the performance of PI with the decline of less than

2 oC. In a word, the thermal stability of PI was not signifi-

cant change with incorporation of GSs. Hence, this rapid

preparation method is a practicable way to prepare excellent

thermal conductivity of composite materials. In addition,

our results also showed that the weight of residue of the PI

composites after pyrolysis is irregular when the GSs content

is higher that 1.0 %, indicating that GSs might facilitate the

flux of the degradation products.

Mechanical Properties of PI Composites. Representa-

tive tensile stress-strain curves and tensile properties of the

neat PI and PI composites for 0.1, 0.5, 1.0, 2.0, 4.0, 7.0, and

11.0 wt% of GSs additives are plotted in Figure 7 and Figure 8.

The tensile specimens are shown in the inset of Figure 7.

From Figure 7, the tensile strength and Young’s modulus of

PI-0.5 increased by 5.8% and 15% in comparison with the

neat PI, respectively. It is attributed to form sea-island struc-

ture of PI composites. PI matrix was the continuous phase,

and the GSs disperse homogeneously in PI matrix, as shown

in Figure 4(b). It is the direct evidence to prove that GSs can

prevent the fracture of PI attributing to the efficient load

transfer from PI to GSs. In addition, GSs can also occur slippage

to dissipate stress to increase the elongation at break. In a

word, the enhancement effect was due largely to good dis-

persion and effective stress transfer. From Figure 8, when

the addition 11.0 wt%, the maximum modulus value is achieved,

up to 4.04 GPa, which is 2 times increase when compared

with the neat PI (2.01 GPa). Meanwhile, the tensile strength

of the PI composites increased with the increase of GSs content

up to 0.5 wt% then decreased with the increase of GSs con-

tent. The maximum value of tensile strength of the PI com-

posites achieved 98.5 MPa with the incorporation of 0.5 wt%.

Figure 5. Thermal diffusivity and thermal conductivity of neat

PI and PI composites with various contents. Figure 6. TGA curves of the neat PI and PI composites.

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Macromol. Res.

Furthermore, the elongation of the PI composites also increased

with the increase of GSs content up to 0.1 wt% then decreased

with the increase of GSs content. The maximum value of

elongation of the PI composites achieved 28.9% with the

incorporation of 0.1 wt% GSs. However, the tensile strength

and elongation of the PI composites decreased with incorpo-

ration of over 0.5 and 1.0 wt%, respectively. It is attributed to

the large agglomerations and cluster of GSs.

Other Properties of PI Composites. Figure 9 shows the

transmittance spectra of neat PI and PI composites with thick-

ness in the wavelength range of 200-800 nm. It can be seen

that the decrease in the transmittance is obvious with increasing

GSs loading, which may be due to too many black GSs in

the composite film. As expected, lower GSs loading composite

films are more optically transparent, with those GSs loading

at 0, 0.1, 0.5, 1.0, 2.0, and 4.0 wt% displaying the optical

transmittances of 76.1%, 63.5%, 11.8%, 4.2%, 3.0%, and 0%,

respectively, at a wavelength of 550 nm. The PI composites

with incorporation of over 4.0% GSs content lose the optical

transparency. The inset of Figure 9 shows the optical images of

neat PI and PI composites with the rectangular of 1 cm×10

cm and the thickness of around 40 μm. It indicates excellent

optical transparency at the lowest weight fractions of GSs.

The hydrophilicity or hydrophobicity is the natural property

of materials. PI film normally exhibits hydrophobicity, whereas

GSs exhibites hydrophilicity due to hydrophilic functional

groups, such as carboxyl groups. In comparison with neat PI

film, the PI composites become more hydrophilic. Figure 10

illustrates the typical appearances of water drop on the PI

film and PI composites. It is obvious that the contact angle

is gradually decrease with those GSs loading increasing.

The hydrophilic behavior could been ascribed as follows: 1)

From the IR spectrum and XPS C1s peaks analysis, it can

be know there are some oxygen-containing groups in the

GSs sheets, which had a certain hydrophilicity. 2) According to

another paper, hydrophilic groups (hydroxyl and epoxy) gener-

ally located in the basal plane of the GSs. One can see from

Figure 3(g) that the higher content of GSs filling had greater

probability to origent along with film surface direction, as a

result of the large aspect ratio of GSs 2D-structure and the

reduced probability of space in perpendicular to the film

surface direction.

Conclusion

PI/GSs composites were prepared by solution blending.

The incorporation of GSs increased the thermal conductiv-

Figure 7. Representative tensile stress-strain curves of neat PI

and PI composites.

Figure 8. Tensile strength, modulus, and elongation at break of

neat PI and PI composites.

Figure 9. Transmittance spectra of neat PI and PI/GSs composite

films. The inset is optical images of neat PI and PI/GSs compos-

ite films.

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Enhanced Thermal and Mechanical Properties of Polyimide/Graphene Composites

Macromol. Res.

ity, thermal stability and mechanical properties of PI. The

thermal conductivity of PI/GSs composites were significantly

improved compared with that of neat PI from 0.254 W/mK

to 1.002 W/mK attribute to the homogeneous dispersion of

GSs and the formation of heat conduction pathway. Further-

more, the Young modulus of PI/GSs was raised up to 4.04 GPa,

approximately a 100% enhancement in comparison with that

of neat PI. In addition, the incorportation of GSs in PI indicated

excellent optical transparency at the lowest weight fractions

of GSs and modified wettability of PI films.

Acknowledgments. The authors gratefully acknowledge

the financial support by National Natural Science Foundation

of China (51303034), the Opening Funding of Guangxi Key

Laboratory for Advance Materials and New Preparation Tech-

nology (12KF-8), Innovation Team of Guangxi Universities’

Talent Highland and Guangxi Funds for Specially-appointed

Expert.

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Figure 10. Photographs of a water drop on the film of neat PI

and PI composites.