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Journal of Mechanical Engineering and Technology 

ISSN 2180-1053 Vol. 13 No. 2           December 2021 

Measurement of Lithium Transference Number in PMMA Solid 
Polymer Electrolytes Doped with Micron-sized Fillers 

R. W. Eric Koh1*, C. C. Sun 1, Y. L. Yap1, P. L. Cheang1, A. H. You1 

1 Faculty of Engineering and Technology, Multimedia University, Jalan Ayer Keroh 
Lama, Bukit Beruang, 75450, Melaka, Malaysia, email: 

ABSTRACT 

PMMA solid polymer electrolytes (SPEs) are much safer than gel polymer electrolytes (GPEs) 
due to their better mechanical and thermal stabilities. In this study, PMMA-LiCF3SO3-EC, 
PMMA-LiCF3SO3-EC-Al2O3 (≤10µm), and PMMA-LiCF3SO3-EC-SiO2 (≤10µm) were prepared 
using solution cast method, their ionic conductivity and lithium transference number was 
investigated using electrochemical impedance spectroscopy (EIS) and Bruce-Vincent method, 
respectively. The experimental result shows that PMMA polymer electrolytes doped with SiO2 
(≤10µm) exhibits the highest ionic conductivity of 2.35×10-4 S/cm and lithium transference of 
0.263 at room temperature. Linear sweep voltammetry (LSV) and Cyclic voltammetry (CV) 
analysis also shows that PMMA SPEs incorporated with SiO2 (≤10µm) fillers can achieve 
electrochemical stability up to 3.2V, exhibits excellent reversibility, and good discharging 
performance.  

KEYWORDS: ionic conductivity; solid polymer electrolyte; transference number; inorganic 
fillers. 

1.0 INTRODUCTION 

Increasing demand and advancement in electronic devices over the years had driven 
forward the development of high-capacity rechargeable batteries and fuel cells. Since the 
first industrial implementation by Sony Corporation in the 1990s, lithium-ion (Li-ion) 
battery has achieved tremendous technological advancement (Osinska, 2009). Their 
contributions, such as larger capacity, higher application voltage, longer lifespan, and 
lower weight, had made them an ideal power source for many applications. Lithium-ion 
batteries can be used in electric vehicles, portable power sources, and space exploration. 
An electrolyte is the heart of a lithium battery, and it acts as a medium for the charge to 
transfer between electrodes.  

However, the liquid and gel electrolyte system in Lithium Batteries (LIB) has potential 
safety issues and poor electrochemical stabilities, which makes them not safe for certain 
applications (Yao, 2019). On the other hand, solid polymer electrolytes (SPEs) are a safer 
alternative. SPEs have better electrochemical stability, environmentally friendly, and 
safer for consumers (Song, 2015; Lim, 2018; Pitawala, 2007). Despite the potential 
advantages, SPEs usage in batteries is hindered due to their high degree of crystallinity 
and high interfacial resistance at ambient temperature, leading to low ionic conductivity 
and lithium transference number.  
PMMA SPEs were a semi-amorphous polymer with improved mechanical and thermal 
properties over GPEs but can still exhibit respectable ionic conductivity and lithium 
*Corresponding author email:1142701349@student.mmu.edu.my

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transference number at room temperature (Sun, 2019; Faridi, 2018). However, most of 
the studies to date were focused on PMMA GPEs, and there are not many studies related 
to PMMA SPEs and their lithium transference number. Faridi et al. investigated the 
electrochemical properties in PMMA-LiClO4 based GPEs for different salt concentrations 
(Faridi, 2018). They achieved an ionic conductivity and lithium transference number of 
12.1×10-3 S/cm-1 and 0.42 respectively for 10% of PMMA and 0.75M of LiClO4. They 
explained that the improvement in lithium transference number is associated with the 
higher polymer content. Higher PMMA concentration improves the degree of 
dissociation of lithium salts in the polymer complexes, frees up Li+ ions for ion 
conduction. 

Musil et al. investigated the lithium transference number using the Bruce-Vincent method 
in PMMA-LiPF6-EC: DMC GPEs with various salt concentrations (Musil, 2014). They 
obtained a lithium transference number of 0.24 and 0.69 for 0.005mol and 1mol of LiPF6 
salt concentration. Hosseinioun et al. also investigated the usage of crosslinked PMMA 
GPEs in Li-ion batteries (Hosseinioun, 2019). They reported that crosslinking increases 
the degree of dissociation of lithium salt in GPEs. The free anions or degree of 
dissociation of lithium salts are higher at 83% in PMMA GPEs than 71% of liquid 
electrolytes, which means PMMA GPEs have better ionic mobility than liquid 
electrolytes. This is evidenced by the obtained lithium transference number of 0.34 for 
PMMA GPEs and 0.24 for liquid electrolytes. 

PMMA GPEs are capable of exhibiting high lithium transference number and ionic 
conductivity at room temperature, but they had poorer mechanical stability and thermal 
stability compared to SPEs. This makes SPEs better canditate for devices that are 
operating in high-temperature environments and require strict safety standards. Thus, in 
this study, PMMA in solid form, a safer alternative, was studied. The ionic conductivity 
and lithium transference number in inorganic filler enhanced PMMA SPEs were 
investigated and compared to results from several literature. Multiple studies have shown 
that PMMA SPEs can be manufactured into solid electrolytes used in supercapacitors and 
li-ion batteries requiring higher safety standards (Lim, 2018; Kurapati, 2019; Zakariya,
2020).

2.0 MATERIAL PREPARATION AND CHARACTERIZATION 

2.1       SAMPLE PREPARATION 

In this study, SPE films were prepared using solution cast method. Poly(methyl-
methacrylate) (PMMA), Ethylene Carbonate (EC), Lithium Triflate (LiCF3SO3), Silicon 
Dioxide (SiO2), and Alumina Oxide (Al2O3) in the experiment were obtained from Sigma 
Aldrich. In a typical synthesis, PMMA, EC, and LiCF3SO3 were dissolved in 
Tetrahydrofuran (THF) and stirred at room temperature for 24 hours until a homogenous 
solution is obtained. The homogenous solution was poured into a petri dish and kept in a 
desiccator until dry electrolytes film of PMMA-LiCF3SO3-EC (SPE1) was obtained. 
Similar steps were used to synthesis PMMA-LiCF3SO3-EC-Al2O3 (SPE2) and PMMA-
LiCF3SO3-EC-SiO2 (SPE3). The prepared sample composition and sample thickness are 
tabulated in Table 1.  

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Table 1. Composition ratio and thickness of PMMA SPE film prepared 

ID 
Weight Percentage wt% 
PMMA EC LiCF3SO3 Al2O3 SiO2 

SPE1 55 18 25 - - 
SPE2 55 18 25 2 (≤10µm) - 
SPE3 55 18 25 - 2 (≤10µm) 

2.2       ELECTROCHEMICAL IMPEDANCE SPECTROSCOPY (EIS) 

Electrochemical Impedance Spectroscopy (EIS) was carried out using Gamry reference 
600 series potentiostat for frequency ranging from 0.1Hz to 1MHz at room temperature 
with the sample sandwiched between two spring-loaded stainless-steel electrodes. The 
ionic conductivity is calculated by using the following equation: 

𝜎 =
𝑡

𝑅!𝐴
(1) 

, where t (cm) is the thickness of SPE film, RB is the bulk resistance of electrolyte obtained 
from the Nyquist plot, and A (cm2) is the contact area between the film and the electrode, 
which equates to 2.56 cm2 in this work. The results of PMMA SPE ionic conductivity 
were tabulated in Table 2. 

2.3       TRANSFERENCE NUMBER CHARACTERISATION 

The lithium transference number was defined as the number of moles of lithium-ion 
transferred for one Faraday of charge transferred. Ideally, the lithium transference number 
should be close to one in a high conductivity lithium polymer battery, and the lithium 
transference number, t+ is calculated as:  

𝑡" =
𝐼#
𝐼$

(2) 

where Io and Is represent the initial and steady-state cell currents, respectively, however, 
the existing system is more complicated, with minute traces of contaminant of oxidation 
on the electrodes that can alter the experiment results. Hence Bruce et al. [12] introduced 
a correction factor to characterize the system before and after polarization, and the 
equation was rewritten as: 

𝑡" =
𝐼#(𝛥𝑉 − 𝐼$𝑅$)
𝐼$(𝛥𝑉 − 𝐼#𝑅#)

(3) 

∆V is the polarization voltage of 20mV, Ro and Rs are the bulk resistance of electrolytes 
film taken into account interfacial resistance before and after the polarization, 
respectively (Bruce, 1987). Thus, the electrolyte film was characterized using EIS before 
and after dc polarization to determine the initial resistance, Ro, and the steady-state 
resistance, Rs of the sample (Pozyczka, 2017).  

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The Bruce-Vincent method is a reliable technique employed by multiple researchers to 
obtain lithium transference numbers in the polymer electrolytes system (Pozyczka, 2017; 
Yang, 2019; Xiao, 2018). High interfacial resistance was always the factor in limiting the 
performance of SPEs. Multiple researchers have reported that interfacial resistance was 
caused by the deposition of the oxide layer resulting from the diffusion of non-lithium 
ions during the chemical reaction. Besides, poor contact between the electrode and 
electrolytes interface, originating from the two different materials mismatched lattice and 
the volume changes occurring during cycling also increase the interfacial resistance 
(Ding, 2020; Jiang, 2019).

2.4       VOLTAMMETRY AND DISCHARGING TEST 

Linear Sweep Voltammetry (LSV) was used to investigate the electrochemical stability 
window of SPEs. The potential window, representing the sample stability voltage, is a 
critical parameter that has to be evaluated to determine the application voltage used in 
electrochemical devices (Aziz, 2019). The voltage was swept from 0V (versus stainless 
steel electrode) at a scan rate of 5mVs-1 until the breakdown of electrolyte films (sharp 
increment of current) to determine the electrochemical stability voltage of the samples.  

Then, five cycles of cyclic voltammetry (CV) were performed on the SPE film from 0V 
to 3V at a scan rate of 20 mVs-1, in which the SPE film was sandwiched between two 
stainless steel electrodes. Lastly, the SPE film was then assembled to evaluate its 
discharge performance. The cell was discharged with a current of 0.01mA at room 
temperature from 2V to 0.1V using stainless steel electrodes. All the measurements were 
carried out using a Gamry Reference 600 series potentiostat. 

3.0 RESULTS AND DISCUSSION 

Figure 1. Nyquist plot of PMMA-LiCF3SO3-EC (Square), PMMA-LiCF3SO3-EC-Al2O3 
(Triangle), and PMMA-LiCF3SO3-EC-SiO2 (Circle). 

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Table 2. Ionic conductivity of PMMA-based solid polymer electrolytes. 

Sample 
ID Sample Composition Filler 

Filler
Size 

Ionic conductivity 
(S/cm) 

SPE1 PMMA-LiCF3SO3-EC - - 1.22 × 10-5

SPE2 PMMA-LiCF3SO3-EC-Al2O3 Al2O3 10 μm 1.83×10-4 
SPE3 PMMA-LiCF3SO3-EC-SiO2 SiO2 10 μm 2.35×10-4 

Figure 1. shows the Nyquist plot for SPE1, SPE2, and SPE3, respectively (see Figure 1). 
The appearance of semicircle for SPE1 suggests the presence of bulk capacitance in the 
system. Simultaneously, the linear line adjacent to the semicircle indicates the diffusion 
process resulting in electrode polarization effect (Saikia, 2008; Sivakumar, 2015). 
Furthermore, no semicircle is observed for SPE2, and SPE3 suggests only resistive 
components prevail. 

The value of bulk resistance was determined at the interception point between the Nyquist 
curve and the x-axis, which corresponds to 964 Ω, and the obtained ionic conductivity is 
shown in Table 2. Ionic conductivity calculated for SPE1 was 1.22×10-5 S/cm. In 
comparison, Pal et al. obtained ionic conductivity of 3.52×10-5 S/cm for plasticized 
PMMA-LiClO4 SPEs (Pal, 2018). Kurapati et al. also reported ionic conductivity values 
of 8.21×10-5 S/cm for her study on PMMA-CH3COOLi SPEs (Kurapati, 2019). The 
obtained ionic conductivity for SPE1 was too low for electrochemical device applications 
(Chauvin, 2006). The low ionic conductivity of SPEs is the attribute of their crystalline 
nature, where the ionic mobility is low. Besides that, most of the Li+ ions already formed 
polymer-salt complexes with the polymer, reducing the fraction of ions available for ionic 
conduction. 

Improvement in ionic conductivity was seen for SPE2 and SPE3 when inorganic fillers 
Al2O3 and SiO2 of (≤10µm) were added, yielding an ionic conductivity of 1.83×10-4 S/cm 
and 2.35×10-4 S/cm, respectively. Chew et al. reported similar findings where they also 
observed improvement in ionic conductivity when they added Al2O3 into PMMA SPEs 
(Chew, 2011). They obtained an ionic conductivity of 2.05×10-4 S/cm for PMMA SPEs 
with Al2O3 fillers, an improvement from 1.36×10-5 S/cm without inorganic fillers. 
Marcinek et al. explained that the improvement in ionic conductivity was associated with 
the increases in conduction pathways for ionic conduction provided by inorganic filler 
due to their larger surface area (Marcinek, 2000). 

Besides that, the presence of inorganic particles in the polymer matrix also lowers the 
fraction of polymer-salt complexes, which increases the fraction of Li+ ions free for ionic 
conduction. Saikia et al. (Saikia, 2008) reported that the glass transition temperature (Tg) 
and crystallinity of P(VDF-HFP)-PC-LiClO4 decreases from -98 ̊ C to -104.6 ̊ C with the 
addition of 4 wt% SiO2 aerogel particles. In Addition, Pitawala also reported decreases in 
Tg from -44 ̊ C to -49 ̊ C when they added 10 wt% of Al2O3 fillers into (PEO)9LiTf 
Furthermore, Dissanayake et al. also reported that the presence of inorganic fillers 
promotes amorphous region in the polymer matrix by lowering the transition temperature 
(Dissanayake, 2003). But they also informed that higher filler concentration above its 
optimal level would impose geometrical constriction, lowering the ion mobility. They 
reported 15 wt% of inorganic filler provided the maximum enhancement. Furthermore, 

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another study conducted by Yang et al. (Yang, 2010) show that decreases in conductivity 
with increasing filler content beyond 2.5 wt% attributed to an aggregation of fillers, 
strongly impeding polymer chain movement. 

Figure 2. DC Polarization curve obtained via chronoamperometry for PMMA-
LiCF3SO3-EC (SPE1) samples. (Inset Nyquist curve of SPE1 before and after dc 

polarization) 

Table 3. Transference number of PMMA-based polymer electrolytes. 

Sample ID Io (μA) Is (μA) Ro (Ω) Rs(Ω)  t+ 
SPE1 0.617 0.055 964.1 1159 0.088 
SPE2 0.834 0.180 69.42 75.31 0.215 
SPE3 1.010 0.266 51.63 81.25 0.263 

Figure 2. shows the current versus time plot obtained using the DC polarization technique, 
the resistance before and after polarization, and the obtained lithium transference number 
was tabulated in Table 3. The measured initial and steady-state currents were used to 
calculate the lithium transference number using Eqn (3) and included in Table 3. The 
lithium transference number obtained for SPE1 is 0.088, which is slightly lower than 0.16 
reported by Xiao et al. for P(VDF-HFP)-LiPF6-EC polymer electrolytes (Xiao, 2018). 
The low lithium transference number reported for SPE1 is associated with insufficient 
free Li+ ions available for ionic conduction due to the formation of polymer-salt 
complexes. 

However, with micron-sized Al2O3 and SiO2 fillers in the polymer matrix, the lithium 
transference number increases up to 0.215 and 0.263 for SPE2 and SPE3, respectively. 
Xiao et al. reported similar findings in their studies where the incorporation of nano-sized 
inorganic fillers enhances the lithium transference number (Xiao, 2018). They obtained a 
lithium transference number of 0.28 to 0.41 at room temperature for P(VDF-HFP) 
polymer electrolytes with 5-15 wt% of nano PMMA-ZrO2 particles, which is an 
improvement from 0.16 without nano PMMA-ZrO2 particles. The improvement in 
lithium transference number is associated with the distribution of inorganic filler in the 
polymer matrix.  

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Firstly, the presence of inorganic fillers reduces the fraction of polymer-salt complexes 
as inorganic fillers such as Al2O3 and SiO2 fillers also forms polymer-ceramic complexes 
with the polymer host. This means that there is more Li+ ions will be available for ionic 
conduction. Besides that, inorganic fillers also promote amorphous region in the polymer 
matrix as they reduced the degree of crystallinity of the polymer chain by lowering the 
glass transition temperature, Tg, which in turn enhances the ionic mobility, thus leading 
to improved lithium transference number. 

Table 4. Lithium transference number obtained in this work compared to other 
researchers. 

Composition Type Reference t+ 
PMMA-LiCF3SO3-EC Solid This work 0.088 
PMMA-LiCF3SO3-EC-Al2O3 (≤ 10µm) Solid This work 0.215 
PMMA-LiCF3SO3-EC-SiO2 (≤ 10µm) Solid This work 0.263 
PMMA-LiClO4-EC Gel Faridi [7] 0.39-0.42 
PMMA-LiPF6-EC Gel Musil [8] 0.24-0.69 
PMMA-LiClO4-PC-EC Gel Appetecchi [26] 0.40 
PMMA-LiBOB-EC Gel Hosseinioun [9] 0.34 
PEO-LiCF3SO3EC-SiO2 (≤ 12nm) Gel Wang [27] 0.54 
PEO-LiBF4-EC-SiO2 (≤ 12nm) Gel Liu [28] 0.34-0.56 
P(VDF-HFP)-LiPF6-EC-PMMA-ZrO2 Solid Xiao [15] 0.28 

Table 4. shows the comparison for the lithium transference number obtained in this work 
to other literature. From the comparison, we can see that PMMA SPEs still have a lower 
lithium transference number compared to GPEs, as reported by (Faridi, 2018; 
Hosseinioun, 2019; Liu, 2004). This is acceptable because GPEs were much amorphous 
compared to SPEs due to their higher liquid solution. However, the higher liquid solution 
in GPEs results in a mechanically soft system and lower thermal stability. Although 
PMMA SPEs incorporated with inorganic fillers has lower lithium transference number 
compared to GPEs, but the presence of fillers in the polymer matrix served as a backbone 
for PMMA SPEs that ensure better mechanical and thermal stability compared to GPEs. 
Liang et al. show that the dispersion of nano-Al2O3 fillers into PEO-PMMA-LiTFSI 
polymer matrix enhances the tensile strength of SPEs up to 3.26 MPA compared to 
2.78MPA for SPEs without inorganic filler (Liang, 2015). 

Nevertheless, the lithium transference number in our study is comparable to the work 
from Xiao et al.. They reported lithium transference number ranging from 0.28 to 0.41 
for P(VDF-HFP) polymer electrolytes doped with nano PMMA-ZrO2 particles, close to 
0.263 obtained for PMMA-LiCF3SO3-EC-SiO2 in our study (Xiao, 2018). The lithium 
transference number in their study is higher than ours because they were using 5%-15% 
of nano PMMA-ZrO2 particles while we only added 2% of SiO2 fillers. Furthermore, the 
nano PMMA-ZrO2 particles also have a greater effective surface area than micron-sized 
SiO2 fillers, which also contributed to the higher lithium transference number obtained in 
their studies. 

Figure 3. shows the LSV plot of the samples. The voltages were swept from 0V (versus 
stainless steel electrode) at a scan rate of 5 mVs-1 until a large increment of current was 
observed (see Figure 3). The large increment in current observed indicates the breakdown 

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of the electrolyte films. The stability voltage can be determined as the intersection of the 
extrapolated linear current in the high voltage region with the voltage axis. 

Figure 3. LSV curves with a scan rate of 5mVs-1 for PMMA-LiCF3SO3-EC (Solid line), 
(b) PMMA-LiCF3SO3-EC-Al2O3 (Dash dotted line), and PMMA-LiCF3SO3-EC-SiO2

(Dash line). 

LSV results revealed that the potential window of the blend is all above 3.0V; SPE1 
(3.07V), SPE2 (3.13V), and SPE3 (3.2V). There was a notable improvement in the SPE 
voltage stability window containing inorganic filler compared to the polymer salts 
system. In comparison, Chandra et al. obtained an electrochemical stability voltage of 
2.69V for PVC-PMMA-LiCl-TiO2 polymer blend, an improvement from 1.69V without 
TiO2 nanoparticles (Chandra, 2017). Dhatarwal et al. also reported stability of 3.0V for 
PEO-PMMA polymer blend doped with various nanoparticles (Dhatarwal, 2018). 

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Figure 4. Five cycles of cyclic voltammetry curve versus stainless steel electrodes with 
a scan rate of 20mVs-1 for (a) PMMA-LiCF3SO3-EC, (b) PMMA-LiCF3SO3-EC-Al2O3

and (c) PMMA-LiCF3SO3-EC-SiO2 
The CV curve of the SPEs was shown in Figure 4. (see Figure 4). The absence of redox 
peak voltages and the overlapping of the subsequent sweeps indicates that the charging 
and discharging reaction at the interface between the electrolytes film and stainless-steel 
electrode is fully reversible for all the SPE films tested (Bandarayake, 2015). Jinisha et 
al. reported CV curve of a similar shape for PEO/PVP-LiNO3 SPEs in their studies 
(Jinisha, 2017). They explained that the missing oxidation-reduction peaks in CV curves 
suggested that the SPE film has great reversibility within the voltage range. Furthermore, 
Bandarayake et al. also reported that CV curves with subsequent overlapping sweeps 
show that the SPE has good cycling capability and a longer lifetime. Their samples can 
retain 96% of its original specific capacity after 20 cycles (Bandarayake, 2016). 

Figure 5. Discharge curve with a discharge current of 0.01mA for PMMA-LiCF3SO3-
EC (black line), PMMA-LiCF3SO3-EC-Al2O3 (red line) and PMMA-LiCF3SO3-EC-

SiO2 (blue line) versus stainless steel electrodes 

Furthermore, PMMA-LiCF3SO3-EC-SiO2 that were doped with SiO2 fillers samples has 
the highest energy density as evidenced by the discharging time as presented in Figure 5. 
(see Figure 5). It can be seen that PMMA-LiCF3SO3-EC-SiO2 takes approximately 16% 
and 190% longer time to discharge compared to PMMA-LiCF3SO3-EC-Al2O3 and 
PMMA-LiCF3SO3-EC, respectively.  

4.0 CONCLUSIONS 

This work provided the ionic conductivity, lithium transference number, and 
electrochemical performance of PMMA SPEs. SiO2 fillers enhanced PMMA SPEs can 
exhibit ionic conductivity of 2.35×10-4 S/cm and lithium transference number of 0.263 at 
room temperature. It is suggested that inorganic fillers promote amorphous region in 
PMMA SPEs, and the greater effective area of the fillers also provides pathways for ionic 
conduction. Besides, the presence of inorganic fillers reduces the fraction of polymer-salt 
complexes, freeing more Li+ ions for ionic conduction. The electrochemical studies also 
show that inorganic filler enhanced PMMA SPEs has great cycling capability and 

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reversibility within a voltage range of 3.0V. Inorganic filler enhanced SPEs may not 
exhibit superb ionic conductivity and lithium transference number like GPEs, but they 
had better mechanical and thermal properties than GPEs, which made SPEs much suitable 
for lower energy density but higher safety applications. 

5.0 ACKNOWLEDGEMENT 

This work is supported by FRGS/2019, Ministry of Higher Education, Malaysia. 

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