International Journal of Polymer Analysis and

Characterization

ISSN: 1023-666X (Print) 1563-5341 (Online) Journal homepage: http://www.tandfonline.com/loi/gpac20

Effects of Ethylene Glycol Dimethacrylate as

Crosslinker in Ionic Liquid Gel Polymer Electrolyte
Based on Poly(Glycidyl Methacrylate)

B.C.F. Wong, A. Ahmad, S.A. Hanifah & N. H. Hassan

To cite this article: B.C.F. Wong, A. Ahmad, S.A. Hanifah & N. H. Hassan (2015): Effects of
Ethylene Glycol Dimethacrylate as Crosslinker in Ionic Liquid Gel Polymer Electrolyte Based on
Poly(Glycidyl Methacrylate), International Journal of Polymer Analysis and Characterization,
DOI: 10.1080/1023666X.2016.1110683

To link to this article: http://dx.doi.org/10.1080/1023666X.2016.1110683

Accepted author version posted online: 26

Oct 2015.

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 Effects of Ethylene Glycol Dimethacrylate as Crosslinker in Ionic Liquid Gel
Polymer Electrolyte Based on Poly(glycidyl methacrylate)

B.C.F. Wong1, A. Ahmad1, S.A. Hanifah1, N. H. Hassan1,

1
School of Chemical Sciences and Food Technology, Faculty of Sciences and
Technology, Universiti Kebangsaan Malaysia, Bangi, Selangor, Malaysia

Corresponding Author. E-mail: syareeda@ukm.edu.my

Submitted: 11 September 2015; Accepted: 16 October 2015.

Downloaded by [University of Nebraska, Lincoln] at 19:52 30 October 2015

Abstract

In this paper, the modified poly(glycidyl methacrylate)-based films for gel electrolyte

were prepared via in-situ UV photopolymerization technique. The effects of adding

ethylene glycol dimethacrylate (EGDMA) into the polymer host were studied through X-

ray diffraction (XRD) analysis and Differential Scanning Calorimetry (DSC). The results

in Fourier Transform Infrared spectra indicate complete polymerization among the

monomers. The addition of EGDMA into the formulation of gel polymer electrolyte

increased the loading of 1-butyl-3-methylimidazolium bis(fluoromethylsulfonyl)imide up

to 200 wt. % with the highest value of 8.2 × 10-4 S cm-1. All the gel polymer electrolyte

membranes obeyed the Arrhenius law.

KEYWORDS: Photopolymerization; Crosslinker; Ionic lqiuid; polymer electrolyte

INTRODUCTION

In the last four decades, solid polymer electrolytes (SPEs) have been widely explored to

replace hazardous liquid electrolytes due to their advantages of flexibility, more safe,

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 ease to fabricate at low cost. SPEs are defined as a polymer-salt complexes in which the

salt is dissolved into the polymer matrix to give a conductive property[1, 2]. Although

SPEs have significantly improved the safety issues of liquid electrolytes, but show low

ambient temperature conductivity which is typically two to four times lower than the

conventional liquid electrolytes[3,4]. In order to possess both cohesive properties of solid

electrolyte and diffusive properties of liquid electrolyte, gel polymer electrolytes (GPEs)

were introduced[5]. The GPEs consist of a larger quantity of liquid electrolyte and
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polymer network, which are completely compatible with each other to form a stable gel[6].

In previous research of GPEs, there were many studies carried out based on poly(ethylene

oxide) (PEO), poly(methyl methacrylate) (PMMA) and poly(vinylidene fluoride) (PVDF)

as polymer supports[7, 8]. Liquid electrolyte trapped in the polymer network can be

designed according to the desired application. For instance, liquid lithium electrolyte has

potential for lithium battery and iodide based liquid electrolyte for dye-sensitized solar

cell applications[9].

There are several techniques used to prepare GPEs. The conventional techniques are

solvent casting and swelling technique[10, 11]. Moreover, GPEs can be prepared by UV

curing which is a well established polymerization technique known as UV

photopolymerization. The multifunctional monomer with appropriate photoinitiator under

exposure to UV light, polymerizes to form polymer films. This technique is solvent free

with low energy consumption and a prompt method[12].

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 Previously, we have reported the preparation of polymer electrolyte based on PGMA-

ionic liquid complexes by using in-situ photopolymerization technique where various

loadings of room temperature ionic liquid (IL) were incorporated into glycidyl

methacrylate (GMA) monomer followed by UV curing to obtain the polymer electrolyte.

However, upon the higher loading of IL, a tacky and non-self standing polymer film was

obtained[13]. Besides, a low loading of IL results in low ionic conductivity. A self-

standing and high ionic conductivity of polymer electrolyte are crucial for energy storage
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application. As reported by Song et al[14], to overcome these problems, either physical or

chemical crosslinking process is required to be implemented during the preparation of

polymer gel electrolytes[15].

The aim of the present work was to modify the polymer network by introducing ethylene

glycol dimethacrylate (EGDMA) as crosslinker in order to improve the physical

appearance and also to increase the loading of ionic liquids as well as the ionic

conductivity of polymer electrolyte membrane. The effects of copolymerizing EGDMA

and GMA monomer were studied. The GPEs were prepared by in-situ photopolymerizing

the GMA-EGDMA monomer mixtures in the presence of a room temperature ionic liquid,

1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide. The maximum loading

of ionic liquid by each sample were reported and the ionic conductivity behavior has been

investigated.

EXPERIMENTAL

Materials

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 Ethylene glycol dimethacrylate (EGDMA), glycidyl methacrylate (GMA), 2,2-

dimethoxy-2-phenylacetophenone (DMPP), chloroform (CHCl3) and 1-butyl-3-

methylimidazolium bis(trifluromethylsulfonyl)imide (BmimTFSI) were purchased from

Sigma Aldrich. All the materials were used without any further purification.

Synthesis

Various amounts of EGDMA (0 to 5 wt. %) were loaded into the 2g of GMA monomer
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mixture which contains an appropriate amount of photoinitiator, DMPP. The

homogenous mixtures were then spread on Teflon plate and followed by UV curing

under nitrogen atmosphere . Clear polymer electrolyte membranes with thickness of 300-

600 µm were obtained.

Characterization

Gel content or insoluble fraction of the cured products was determined by the chloroform

extraction method. Samples were contained in a metal net and immersed in CHCl3 for 72

hours at room temperature to dissolve non-crosslinked products. The gel content was

calculated by dividing the mass of dry sample by the mass of the original sample (relative

error = ± 1%)[9,16-17].

Chemical interaction between crosslinker and GMA was investigated through ATR-FTIR

analysis. The samples were tested by using Spectrum 400 Perkin Elmer GX Spectrometer

in the frequency range of 4000 to 650 cm-1.

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 Crystallinity and structure of the polymer films were studied by X-ray diffraction (XRD).

This measurement was conducted by Bruker D8-Advance diffractometer with the

diffraction angle, 2θ range of 10 º to 80 º at a scanning rate of 0.025 º s-1.

Glass transition temperature (Tg) of the prepared polymer films was determined by using

DSC 822 Mettler Toledo. The samples were loaded and cooled to 0 ºC and heated with a

heating rate of 10 ºC/min to 150ºC. The Tg was taken at the midpoint of the heat capacity
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change from the amorphous glassy state to rubbery state.

To understand the holding power of the polymer matrix after loading various amounts of

crosslinker, ionic liquid BmimTFSI as liquid electrolyte was loaded into the polymer

matrix by one pot in-situ photopolymerization process to form polymer gel electrolyte

films.The polymer gel electrolyte films with its maximum loading of BmimTFSI were

tested by HIOKI 3532-50LC HiTester impedance analyzer to determine the ionic

conductivity. The prepared films were sandwiched between two stainless steel electrodes

with the effective surface area, A of 1.76cm2. Ionic conductivity, σ, was calculated using

the equation σ = tRb-1A-1, where t represents the thickness and Rb is the bulk resistance

of the samples.

RESULTS AND DISCUSSION

3.1. The Properties Of EDGMA Incorporated PGMA Films

To prepare the UV-crosslinked polymer films, various amounts of EGDMA were loaded

into GMA monomer mixtures which contained photoinitiator to form homogenous

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 mixtures and followed by UV curing. Under UV irradiation, radical was generated from

DMPP to initiate polymerization (Scheme 1). Random copolymerization happens

between the GMA and EGDMA. GMA as monofunctional monomer contributes to the

propagation of the chain during the photopolymerization process, meanwhile EGDMA as

multifunctional monomer builds the three-dimensional network[17, 18]. After UV curing,

the monomer mixtures were transformed into a clear, transparent and rigid polymer film.

The composition and the designation of the polymer films are given in Table 1. Sample
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CL-0 without EGDMA dissolved thoroughly in the chloroform. As the loading of

EGDMA increased, gel content of polymer films increased. This indicates that the

polymer chains in films are crosslinked with the presence of EGDMA. Due to the high

gel content, the sample CL-1 to CL-5 are not dissolved in most of the solvents such as

toluene, tetrahydrofuran, dichloromethane, ethanol and methanol to form a homogenous

solution. Furthermore, a highly crosslinked polymer cannot swell or absorb much liquid

due to its limited segmental motion[19].

The Tg of the prepared polymer films was shown in Table 1. Sample CL-0 shows

the glass transition temperature at 60 ºC. After adding the crosslinker, Tg shows a slight

decrease. There is not much differences after adding 1 to 5 wt. % of EGDMA into the

polymer films. This may be due to the presence of small amount EGDMA in polymer

matrix which does not affect much on the Tg.

The chemical structures and the nature of bond formations in the polymer matrix

were illustrated by using ATR-FTIR spectroscopy analysis. By referring to molecular

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 structures of EGDMA and GMA in Scheme 1, both of them possess similar functional

group except the epoxy group. In Figure 1, both GMA and EDGMA revealed alkene

C=C-H bending, C=C twisting vibration band and stretching band at the same

wavenumbers of 942, 814 and 1637 cm-1 respectively. Another significant sharp peak

appears in IR spectra of GMA and EGDMA at the wavenumber of 1716 cm-1 assigned to

the C=O ester stretching band. Besides, a strong stretching band of C-O-C ether group

was observed at 1140 and 1154 cm-1 respectively for EGDMA and GMA monomers[20,
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21]
.The peaks of epoxy group of GMA appeared significantly at 1294, 907, 842 and 761

cm-1 which is attributed to weak ring stretching band, asymmetric and symmetric

stretching and lastly C-H bending vibration of epoxy group[13, 22-23].

After the UV photopolymerization process, GMA monomer copolymerized with

EGDMA crosslinker to form polymer film. The formation of the polymer chains is based

on free radical mechanism through the C=C alkene group. Through Figure 1(c) and (d),

CL-0 and CL-5 showed a similar IR absorption pattern. For both spectra of CL-0 and CL-

5, the signals related to C=C alkene group at 814, 942 and 1637cm-1 disappeared. This

clearly indicates the completion of radical photopolymerization process. The presence of

the epoxy band in Figure 1 (c) signifies that there is no ring opening of the epoxy ring to

form a new crosslinking point[24]. Furthermore, C=O ester band was shifted from 1716 to

1721 cm-1 due to the missing of C=C bond of methacrylate. During the

photopolymerization, the double bond alkene group of methacrylate will transform to

single bond –CH2 alkane group which exists at 991 cm-1 as –CH2 wagging mode. In other

words, the α,β-unsaturated ester group of GMA and EGDMA monomer has transformed

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 to the saturated ester group after the polymerization. Usually, α,β-unsaturated ester group

will exist at lower wavenumber due to the resonance effect.

XRD analysis was used to further understand the structure of the polymer films after the

addition of crosslinker into the PGMA polymer system. The presence of broader peaks in

diffractogram has proven that the prepared polymer films exist as semi-crystalline. In

Figure 2, the pristine PGMA (CL-0) showed three intense peaks in the region of 5-25º,
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25-35º and 35-45º[25]. Poly(EGDMA) was the polymer synthesized by using EGDMA

monomer through UV photopolymerization technique. It revealed a small hump in the

region of 10-25º. Sample CL-1 to CL-5 showed similar X-ray diffractogram as in Figure

2 which shows a less intense peak in a region of 12-25º compared with CL-0. Although

the amount of EGDMA added was just 5 wt. % of GMA monomer, it affected the

structure of the PGMA matrix by reducing the overall crystallinity. Based on the result

of XRD analysis, the EGDMA does play its role as a crosslinker to build up a crosslinked

PGMA matrix which crystal molecules are less closely packed together in order

compared with the pristine PGMA matrix. This is in agreement with Nair et al[26], who

described that the crosslinked polymer is more amorphous compared with the non-

crosslinked polymer.

3.2 Bmimtfsi Incorporated Polymer Electrolyte and Ionic Conductivity Study

In our first attempts to synthesize the polymer gel electrolytes, we adopted the swelling

method to incorporate BmimTFSI as electrolyte into polymer matrix. By using this

method, BmimTFSI uptake is low and inquires longer time[12]. Therefore, we solved this

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 problem by curing the homogenous monomer mixture in the presence of BmimTFSI with

UV light. By this method, we were able to load BmimTFSI into the polymer films and

the holding strength of each sample was studied. Instead of rigid polymer films,

mentioned in previous sections, clear, transparent,flexible and self-standing polymer

films are obtained (Figure 3). This is due to the plasticizing effect of BmimTFSI which

transforms the structure of semi-crystalline to fully amorphous[13].

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The loading of BmimTFSI varies from 0 to 200 wt. % of monomer. It is interesting that

the polymer films with different amount of crosslinker have different holding power as

shown in Figure 4. The sample without crosslinker (CL-0) can only hold maximum 70

wt.% of BmimTFSI, the overloading of BmimTFSI results in tacky and non-self standing

films. The addition of EGDMA improved the holding power of the polymer films. We

found that samples CL-1, CL-2 and CL-3 were capable to hold maximum 100 and 160

wt. % of BmimTFSI respectively. CL-4 and CL-5 were able to hold more than 200 wt. %

of BmimTFSI but the further incorporation of BmimTFSI does not increase much in the

ionic conductivity, thus we stoped the loading at 200 wt. %. As illustrated in Figure 5(a),

CL-0 without crosslinker forms linear homopoly(GMA) chains within the polymer-

BmimTFSI complex. In the absence of crosslinker, there are only relatively weak inter-

polymer chain bonds such as Van Der Waals and hydrogen bonds that hold the polymer

chain and IL together in solid state[27]. Hence, CL-0 can only hold 70 wt.% of

BmimTFSI. Figure 5(b) isassigned to samples CL-1 to CL-5 which consist of crosslinked

PGMA chains in its polymer-BmimTFSI complexes. EGDMA built up the bridges

between the linear polymer chains to form a three-dimensional network that prevents the

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 chain separation and increases the holding strength of the polymer matrix. Consequently,

with the aid cross-linkable moieties, a higher IL content can be loaded into polymer

matrix without losing the mechanical stability[28].

Ionic conductivity, σ is calculated by the equation: σ = where n is the number of

charge carrier, z assigned to ionic charge and µ presents the ionic mobility. BmimTFSI

consists of Bmim+ and TFSI- ions that incorporated into the polymer matrix play the role
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of charge carrier. Hence, the increment of the IL loading results in the enhancement of its

ionic conductivity as shown in Figure 4. CL-0 with 70wt.% BmimTFSI gives only 3.1 ×

10-6 S cm-1 meanwhile CL-1 with 100wt. % BmimTFSI gives 5.2 × 10-5 S cm-1. CL-2 and

CL-3 show the conductivity of 5.3 × 10-4 and 4.3 × 10-4 S cm-1 respectively. Both CL-4

and CL-5 that hold 200 wt.% of BmimTFSI possess the conductivity of 7.6 × 10-4 and

8.2 × 10-4 S cm-1. Both pristine and crosslinked PGMA films itself show a conductivity

value of 10-11 S cm-1. The enhancement of ionic conductivity, in particular at room

temperature, increased 5 orders ofnmagnitude for CL-0, 6 orders magnitude for CL-1 and

lastly 7 orders magnitude for CL-2 to CL-5. Significantly, after the uptake of 160 wt.% of

BmimTFSI, there is no drastic increment of ionic conductivity.

The temperature-dependent ionic conductivity of the polymer gel electrolyte, CL-5 with

200 wt. % was studied. The ionic conductivity of the polymer gel electrolyte increases

with the temperature as shown in Figure 6. At 363K, the ionic conductivity values as high

as 5.0 x 10-3 S cm-1. A linear plot was found between conductivity and temperature with

the regression coefficient of 0.9996 based on the Arrhenius law :σ = σ ο е(-Ea/KT), where

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 σ ο assigned to pre-exponential factor, Ea is activation energy, K is Boltzman constant

and lastly T is the temperature in Kelvin[29,30]. This indicates that the polymer gel films

exhibit Arrhenius-like behavior where the Bmim+ and TFSI- ions dissociated and revealed

ionic hopping mechanism in the crosslinked PGMA-IL complexes[31]. From the plot, Ea

was calculated and showed the value of 0.32 eV .

CONCLUSION
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The addition of only 4 wt. % EGDMA into the formulation of preparing PGMA polymer

films has successfully improved the gel polymer electrolyte by increasing the uptake of

BmimTFSI up to 200 wt. % whilst preserving the physical appearance. Via in-situ

photopolymerization technique, flexible and self-standing polymer films were obtained.

The higher loading of EGDMA incorporated into the polymer matrix, the higher the gel

content is due to the formation of cross-linkage between the PGMA chains. The Tg of the

crosslinked PGMA films was lower compared to pristine PGMA films. Based on XRD

analysis, the crosslinked PGMA films are more amorphous compared to pristine PGMA

films. The sample CL-5 with the loading of 200 wt. % revealed the ionic conductivity as

high as 8.2 × 10-4 and 5.0 x 10-3 S cm-1 at ambient temperature and 363 K respectively.

ACKNOWLEDGEMENTS

This work was supported by Exploratory Research Grant Scheme

(ERGS/1/2013/TK07/02/4) and ETP-2013-027. Besides, the authors sincerely gratitude

to Centre for Research and Instrumentation Management (CRIM) for the technical and

analytical study supports.

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 Table 1. The gel content of the PGMA films with different loading of EGDMA according

to its designations.

Designations Composition of EGDMA Gel content (%) Tg (ºC)

(wt. %)

CL-0 0 0.0 60

CL-1 1 73.9 57

CL-2 2 88.8 56
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CL-3 3 89.4 56

CL-4 4 92.8 57

CL-5 5 94.9 58

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 Figure 1. ATR-FTIR spectra of (a) EGDMA monomer, (b) GMA monomer and (c) CL-0

and (d) CL-5

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Figure 2. X-ray diffractrogram of the different samples as labeled
 Figure 3. Physical appearance of sample CL-5 loaded with 200 wt. % of BmimTFSI.
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 Figure 4. The maximum loading of BmimTFSI and its ionic conductivity in different

samples measured at ambient temperature.

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 Figure 5. Schematic illustration of (a) non-crosslinked and (b) crosslinked BmimTFSI-

incorporated PGMA electrolytes.

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 Figure 6. Arrhenius plot of CL-5 containing 200 wt. % BmimTFSI measured from 303K

to 363K.
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 Scheme 1. Propagation reaction of (a) GMA monomer to form a linear homopolymer

chain and (b) copolymerization between GMA and EGDMA with the formation a three-

dimensional crosslinked network.

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