Journal of Sustainability Science and Management eISSN: 2672-7226

Volume 16 Number 3, April 2021: 91-102 © Penerbit UMT

IMPROVING PERFORMANCE OF LEAD-ACID BATTERIES THROUGH

CARBON LEAD HYBRID ELECTRODES

VAN MEN TRUONG*1, NGOC BICH DUONG2, TRAN VAN DIEN1 AND HUYNH THANH
BANH1
1
School of Engineering and Technology, Tra Vinh University, 126 Nguyen Thien Thanh Street, Ward 5, Tra Vinh 87000,
Vietnam. 2School of Agriculture and Aquaculture, Tra Vinh University, 126 Nguyen Thien Thanh Street, Ward 5, Tra Vinh
87000, Vietnam.

*Corresponding author: [email protected]

Submitted final draft: 18 June 2020 Accepted: 25 June 2020 http://doi.org/10.46754/jssm.2021.04.008

Abstract: This paper presents the study of the addition of carbon materials to negative
electrodes to upgrade the performance of lead-acid batteries through avoiding sulfation
and getting super capacitance effects due to their high specific surface area. Two kinds of
carbon materials including carbon fibre paper and activated carbon cloth with high electrical
conductivity and porosity are selected in the experiments. The required hydrophilicity of the
carbon materials is pretreated and checked through the surface contact angle measurement
before added. The surface morphology of carbon materials, negative electrodes are also
observed using Scanning Electron Microscope. The results show that the performance of
the carbon-added battery cells is improved. The initial capacity and specific energy of
the tested battery cells with the carbon cloth addition are about 15% higher than those of
battery cells without the carbon addition. Moreover, the lead sulphate crystal size formed
on the negative electrode surfaces of the carbon added batteries are smaller than that on the
negative electrode surfaces of the conventional batteries, revealing that carbon addition can
improve the battery lifespan.

Keywords: Lead-acid battery, battery performance, carbon lead hybrid, carbon material.

Introduction the electrolyte (sulfuric acid). The chemical

Lead-acid batteries are the most used reactions take place at anode and cathode during
battery in automobile, transportation and the charge/discharge processes as follows
telecommunication industries. They basically (Zimáková et al., 2015) (note that the upper
consist of sponge lead plates (negative arrow represents the direction of the reaction
electrodes), separator (insulation material), during discharging and the lower arrow while
lead dioxide plates (positive electrode), and charging):

(1)

(2)

(3)

With advanced technology, to provide the which can’t be converted successfully back
power capability and adequate service-life in to spongy lead during the charging process,
advanced systems, lead-acid batteries should leading to battery failure (Lam et al., 2004). In
work as effectively as possible under high-rate, recent years, many researchers are interested in
partial-state of charge/discharge (HRPSoC) improving performance and cycling life of lead-
conditions that quickly cause the accumulation acid batteries in order to meet the demands of
of lead sulfate (PbSO4) on the negative plates modern applications.
Van Men Truong et al. 92

Many attempts have been carried out, content of graphite and black carbon was the
and it is found that adding carbon to lead- same amount of 2wt.% (Boden et al., 2010).
acid electrodes during paste preparation in a In addition, the maximum cycle number was
variety of forms, including activated carbon, achieved at low concentration of graphite
carbon black, graphite and carbon nanotubes, (near 1~1.5 wt.%) added to negative plates
can enhance both performance and lifespan of as observed by some other researchers (Bača
the batteries. In particular, Shiomi et al. (1997) et al., 2011; Soria et al., 2005). Blecua et al.
investigated the benefits of carbon added to the (2017) investigated the influences of different
negative active material (NAM). They proposed carbon materials on lead-acid batteries used
that the advantages were caused by a conductive for micro-hybrid vehicles. They reported that
network of carbon particles formed on PbSO4 carbon materials with big particle size were able
crystals leading to the improvement of cycle to improve cycle life and charge acceptance
life performance. Their opinion was later agreed while carbon black with small particle size (<1
by Ohmae et al (Ohmae et al., 2003). They μm) may increase water consumption and fail
also suggested that highly conductive carbon to prolong cycle life. In addition, the effects of
should be used to retard the sulfation process. specific surface area (SSA) and morphology of
Pavlov et al. (Pavlov et al., 2009) discovered different carbon materials added to the cathode
that the electrochemical reaction of lead ions electrode of lead-acid battery were explored
occurs simultaneously on both surfaces of Pb by Hu et al. (2019). Carbon materials with
and carbon particles during the cycling of cells. larger SSA and smaller carbon particle size are
A parallel electrochemical mechanism was also beneficial for enhancing battery performance.
proposed based on their experiments. Xiang’s The former can enlarge the electrochemical
group (Xiang et al., 2013) has pointed out that active surface of the active material while the
the roles of carbon additives to negative plates latter is more effectively dispersed within the
under HRPSoC duty can be summarized from active materials. Besides, Yin et al. (2018)
three aspects: (i) increasing the porosity and also demonstrated that high reversibility of the
active surface area of NAM due to formation of anode and low hydrogen evolution of lead-acid
a new porous-skeleton builder; (ii) facilitating battery can be achieved by grafting lead on the
electrolyte diffusion from the surface to the anode C/Pd composite. They concluded that
inner of plates; (iii) sharing excess charge the main roles of C/Pd composite in the anode
and discharge current with negative plates. includes maintaining a solid anode structure
Sugumaran et al. (2015) demonstrated that with high specific surface area and enhancing
the incorporation of discrete carbon nanotubes charge acceptance. In their latter work (Yin et
(dCNT) was useful not only in negative plates al., 2019), the optimized composition of C/Pd
but also in positive plates. Cycle life tests of was also obtained. The results showed that the
the batteries increased more than 60% as the cycle life of the battery cell with the addition of
negative plates were accompanied by dCNT optimized C/Pd composite to the negative plate
while it was significantly improved by 500% in is about 11 times longer than that of the blank one
the case of both electrodes added. The dCNT/ under HRPSoC. Carbon material addition can be
Had overcharge reaction mechanism was also designed to provide super capacitance effects.
proposed to explain their observation. A similar Particularly, Lam et al. (Lam et al., 2006; Lam
observation when adding carbon materials to et al., 2007) have developed the ultra-battery
anode and cathode electrodes was also reported with a conventional PbO2 positive plate and a
by Lang et al. (2018). Furthermore, the impact negative plate consisting of two parts: half of it
of different types and concentrations of carbon is a sponge lead material and the other half is a
materials have been studied as additives in carbon electrode. Their results showed that the
lead-acid batteries. Cycle life under HRPSoC performance of the ultra-battery increased by
operation was enhanced as the optimized 50% and its cycle life is significantly improved

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IMPROVING PERFORMANCE OF LEAD-ACID BATTERIES THROUGH CARBON LEAD 93

compared to the conventional lead-acid battery. make manufacturing processes of lead-acid

The carbon electrode in the ultra-battery design batteries more complex. Therefore, in this work,
acts as an asymmetric supercapacitor which is a simple approach without elaborate synthesis of
able to provide and rapidly absorb charge during composites and surface chemistry modification
HRPSoC operations. The application of the is studied for improving the capacity and cycle
ultra-battery design for a fuel cell hybrid vehicle life of conventional lead-acid batteries. Highly
was then numerically investigated (Huang et porous and electrically conductive carbon
al., 2016). By applying a lithium battery and materials under the form of fiber paper or cloth
the ultra-battery as auxiliary power sources are prepared and directly added in parallel to the
in the fuel cell hybrid vehicle module, the negative plates of an assembled 2 V lead-acid
simulation results showed that the power output cell with two positive plates and three negative
curves of the ultra-battery and lithium battery plates that are separated by absorbed glass-mat
are extremely similar, while the cost of ultra- (AGM). The carbon interlayer is expected to
batteries is competitive with the lithium battery. provide the electrically conductive network on
Carbon fiber papers or carbon clothes are the negative electrode surface and the super
currently the most common materials used capacitance effect which not only acts to limit
to make gas diffusion layers (GDL) in fuel or the formation of hard sulfation inside the cell
biofuel cells (Zhang et al., 2002; Liu et al., but also increases its charge acceptability. The
2009; Zhang et al., 2017). In addition, it is also ratio of the surface area of carbon sheets to
preferred for use in supercapacitors as electrodes negative plates is 1:2 or 1:1. The contact angle
(Shang et al., 2017; Bavio et al., 2017; Wang et measurement, SEM, and chronopotentiometry
al., 2016; Li et al., 2017) because they possess are employed for the characterization of carbon
the advantages of good conductivity, porous materials, carbon lead hybrid electrodes and
form, high specific surface area, corrosion constant current discharge in this investigation.
resistance, stability, and moderate cost. In
the last two decades, the advantages of using Materials and Methods
carbon papers or carbon clothes instead of using
Preparation and Characterization of the Added
metallic alloy in lithium-ion batteries have been
Carbon Materials
discovered by many research groups (Su et al.,
2012; Isaev et al., 2003; Arbizzani et al., 2005; Carbon fiber papers and activated carbon clothes
Arbizzani et al., 2006). As carbon papers were (produced by CeTech, Taiwan) with thicknesses
used as a substrate-current collector, it enhanced of 0.60 mm and 0.65 mm were used in this study
not only constant capacity but also cycle life due as shown in Figure 1(a) and (b), respectively.
to the flexible property of carbon materials which The specific surface area and porosity analysis
provides good contact with the cathode surface, for the prepared samples were characterized
offering electron pathways during lithiation/de- by N2-adsorption/desorption isotherms at 77K
lithiation (Arbizzani et al., 2005; Arbizzani et (ASAP 2020, Micromeritics, USA). The pore
al., 2006). When the microporous carbon paper volume and pore size were calculated according
was inserted between cathode and separator, it to the method of BJH (Barrett Johner Halenda).
decreased the internal charge transfer resistance The characteristics of the carbon paper and
and captured the migrating polysulphides during activated carbon cloth are summarized in Table
electrochemical reactions. 1. The results show that the specific surface area
and pore volume of the activated carbon cloth
From earlier studies, it is obvious that
are larger than those of the carbon fiber paper.
the addition of carbon materials can enhance
The estimated average pore size for the activated
the performance and prolong the cycle life of
carbon cloth (115.036 Å) is also much greater
lead-acid batteries. However, mixing carbon
than that of the carbon fiber paper (20.927 Å).
powder with active electrode materials will

Journal of Sustainability Science and Management Volume 16 Number 3, April 2021: 91-102
Van Men Truong et al. 94

Figure 1: Carbon materials: (a) Carbon fiber paper and (b) Activated carbon cloth

Table 1: Specific characteristics of carbon materials used in this study

BET surface Pore area Pore volume Average pore

Carbon type
area (m2/g) (m2/g) (cm3/g) size (Å)

Carbon fiber paper 1.4773 1.2845 0.000672 20.927

Activated carbon cloth 1.6006 1.4695 0.004226 115.036

Preparation of the Negative and Positive Plates

In this study, the positive plates and negative
plates mainly made of lead dioxide and sponge
lead, respectively, were all produced by Taiwan
KUNG LONG batteries industrial CO., LTD.
The areal loadings of the negative plate, positive
plate, and AGM separator are 1.06, 1.09, and
0.064 g cm-2, respectively. The sizes of the
negative and positive electrodes are 75 mm ×
37 mm × 1.8 mm and 75 mm ×37 mm × 2.0
mm, (height × width × thickness), respectively.
Absorbent Glass Mats (AGMs) with a size of 80
mm × 40 mm × 3.0 mm were used to separate
the positive plates and negative plates. The
electrolyte was H2SO4 with a density of 1.28 g/
cm3 (Yang et al., 2017) used during all tests. The
real battery cell is presented in Figure 2.

Figure 2: The actual battery cell used in this work

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IMPROVING PERFORMANCE OF LEAD-ACID BATTERIES THROUGH CARBON LEAD 95

Design of the Tested Lead-Acid Cells comparison, a 2 V cell consisting of the same
The influence of the addition of carbon fiber negative and positive plates without carbon
paper and activated carbon cloth to negative sheet addition was also produced.
plates on battery performance was investigated
in 2 V test cells. The schematic of the test cells Capacity Test
is shown in Figure 3. In each 2 V test cell, For this test, fully charged battery cells were
three negative plates were assembled with two discharged to the final voltage of 1.6 V (cut-off
positive plates and AGM separators with a voltage) at a constant current of 0.5 A. The cells
thickness of 3.0 mm. The prepared carbon papers were then charged for 12 h at a constant voltage
or cloth were manually introduced to the cell. of 2.5 V with a current limit of 0.25 A. These
In particular, three negative plates electrically cells were subsequently cycled. All the tests are
connected by bridge weld were interlaced with carried out at room temperature (~25 oC). The
two positive plates electrically connected in capacity and specific energy of the tested battery
the same manner. After that, Absorbent Glass cells were calculated from the following Eqs. (4)
Mat (AGM) and carbon fiber paper or cloth, and (5).
prepared to the proper sizes, were inserted into
(4)
the gap between the negative and positive plates,
where the carbon fiber was contacted with the
negative plates as shown in Figure 3. The ratio (5)
of the surface area of the carbon material to the
negative plate was 1:2 or 1:1 (50% or 100%, where: C is the capacity (Ah); Es is the specific
defined as insertion ratio). The designed cell energy (Wh/kg); I, U(t), t, and m are the discharge
was placed inside a plastic container provided current (A), discharge voltage, discharge time
by the supplier (Taiwan KUNG LONG (h), and mass of battery cell (kg).
batteries industrial CO., LTD). Subsequently,
the electrolyte (H2SO4) was introduced to the Results and Discussion
cell from the top. After that, the cell was sealed
with a top cover and sealing glue to form a sealed Carbon fiber paper and activated carbon cloth
lead-acid battery. The positive and negative were required to have hydrophilic characteristics
terminals were exposed outside the top cover in order to make H2SO4 solution or water easily
for charge and discharge processes. There was a penetrate these layers. However, by using
safety valve on the cover designed to release any Optical Contact Angle Meter Model 100SB, the
excess pressure if the battery is overcharged. As original carbon fiber papers and activated carbon
a result, the loss of H2SO4 in the sealed lead acid cloth were hydrophobic with the surface contact
battery cell can be significantly diminished. For angle of 129.99o and 124.60o, respectively, as

Figure 3: Schematic of the tested lead-acid cell: (a) 50%; (b) 100%

Journal of Sustainability Science and Management Volume 16 Number 3, April 2021: 91-102
Van Men Truong et al. 96

depicted in Figures 4(a) and (b). To form the charging, due to the supper capacitance effect
hydrophilic functional group (COOH), they of the inserted carbon materials (Lam et al.,
were immersed in the mixture of concentrated 2007; Huang et al., 2016; Smith et al., 2002).
acids (H2SO4: HNO3 = 3:1) for 10 minutes with In other words, with carbon fiber addition, a
sonication to produce carboxylic acid group super capacitor is formed based on one lead-
(COOH) (Zhang et al., 2008). The contact angle dioxide positive plate and one carbon-based
measurement of the treated carbon materials negative plate. As a result, during the charging
was then observed. As shown in Figures 4(a1) process, a certain amount of charge will be
and (b1), after modification, a droplet of contact electrostatically stored on the carbon plates and
angle measurement was immediately absorbed release this additional charge in the discharge
once it reached the carbon paper or carbon cloth process, improving the cell capacity. The second
surfaces. Water was evenly laid on the surfaces benefit is enhancing electron conductivity on the
and it is defined as the contact angle 0°. In negative electrode surfaces due to a conductivity
other words, the hydrophilicity of the modified network formed by the carbon plates (Moseley
carbon materials meets the requirement for this et al., 2006). During discharging, the partial
investigation. transfer of electrons generated on the negative
Figure 5 shows the discharge curves of electrode surface can be implemented through
the batteries with and without adding carbon the carbon plate, helping the sponge lead react
materials at a constant discharge current of 0.5 with HSO4- to evenly form PdSO4 on the negative
A. It is observed that the discharge time of the surface. Conversely, in the charging process, the
battery cells with carbon fiber paper or activated external electrons are partially transferred from
carbon cloth is longer than that without carbon the carbon plate to the negative plate, making
addition, indicating that the performance of the a better dissolution of PdSO4. Accordingly, the
carbon-inserted battery cells is improved. The reversibility of the charging and discharging
initial capacity and specific energy of the tested processes is improved. The results also show
battery cells were also calculated and presented that the larger an area of carbon materials was
in Table 2. With carbon insertion, the initial added, the better battery performance was
capacity and specific energy of the tested batteries achieved. This makes sense, because more
increase. It is expected that the presence of the charge will be stored on the larger carbon
carbon pieces could have two main benefits. The surface area. In general, a higher insertion ratio
first is increasing the charge acceptance during is also beneficial for both conductive network

Figure 4: Contact angle measurement of carbon fiber paper: (a) before modification; (a1) after modification
and of activated carbon cloth: (b) before modification; (b1) after modification

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IMPROVING PERFORMANCE OF LEAD-ACID BATTERIES THROUGH CARBON LEAD 97

formation and supercapacitance effect, leading better conductive network for electrons transfer
to better battery performance. The highest during chemical reactions while the second
improvement of the specific energy of the tested one will provide large gravimetric capacitance
battery cell with the insertion ratio of 1:1 of the and hence energy storage density (Zhang et al.,
activated carbon cloth is around 15% compared 2013; Ji et al., 2014). The reported improvement
to the conventional battery cell. Furthermore, the of lead-acid battery performance using different
addition of activated carbon cloth exhibits better carbon materials as additives is summarized in
initial capacity and specific energy than that of Table 3. It can be seen that our lead-acid battery
carbon fiber paper. This could be due to activated cell with carbon-lead hybrid negative electrodes
carbon cloth possessing higher flexibility and exhibits a comparable initial capacity, as
larger specific surface area (as presented in compared with the previously reported results in
Table 1) compared with the carbon fiber paper. lead-acid battery researches, suggesting that the
As a result, the first property will make better carbon fiber insertion to the negative electrodes
contact between the carbon cloth surface and can be used for improving the performance of
negative electrode surface, which provide a conventional lead-acid batteries.

Figure 5: Discharge curves of the tested battery cells

Table 2: Initial capacity and specific energy

50% 100% 100%

50% carbon
carbon carbon carbon
Tested Cell Bare lead paper
cloth paper cloth
inserted
inserted inserted inserted
Initial Capacity (Ah) 3.76 ±0.11 3.98 ±0.13 4.25 ±0.10 4.21 ±0.14 4.32 ±0.13
Specific energy 36.16
32.03±0.11 33.90 ±0.12 36.02 ±0.14 36.88 ±0.12
Wh/kg ±0.10
Improved capacity
- 5.9 13.2 12.0 14.9
(%)
Improved specific
- 5.8 12.9 12.5 15.1
energy (%)

Journal of Sustainability Science and Management Volume 16 Number 3, April 2021: 91-102
Van Men Truong et al. 98

Table 3: Reported improvement of lead-acid batteries using different carbon materials as additives

Improved percentage of initial

Discharge rate Reference
capacity (%)
0.05C 23.5 (Saravanan et al., 2012)
0.5C 3.5 (Hong et al., 2014)
0.5C 10.7 (Kumar et al., 2014)
1C 26.7 (Zou et al., 2014)
0.1C 5.5 (Saravanan et al., 2015)
0.1C 19.9 (Lang et al., 2018)
0.1C 14.9 (Yin et al., 2019)
1.8C 11.5 (Hu et al., 2019)
0.125C 14.9 This work

To observe the lead sulfate crystals on capacity of the lead-acid batteries with added
the negative electrodes after discharging, the carbon cloth is achieved compared to the lead-
negative electrodes were rinsed in several baths acid batteries with added carbon fiber paper. The
of deionized water and scanned using SEM surface area and porosity measurements for the
(Hitachi model S-3400N). The SEM images of negative electrodes will be conducted in future
different negative electrode surfaces are shown work.
in Figure 6. It can be observed that the size of
the lead sulfate crystals on the carbon added
Conclusion
negative electrode surfaces are smaller than
those on the bare negative electrode surfaces. A simple method to boost the performance
This is because the added carbon materials can of lead-acid batteries has been proposed and
facilitate the formation of small isolated PbSO4 experimentally studied in this work. The
particles which are easy to dissolve and restrict results show that the lead-acid batteries exhibit
PbSO4 crystal growth (Shiomi et al., 1997). The improved performance when carbon paper or
results indicate that the lifespan of battery cells carbon cloth is added to the negative electrode
with carbon materials inserted could be improved surfaces. The initial capacity of the battery with
compared to the original battery cells since the 100% carbon cloth insertion increases by 15%
larger lead sulfate crystals are harder and cannot compared to the original lead-acid counterpart.
be completely converted back to sponge lead Additionally, morphology analyses of negative
during the charge process (Sugumaran et al., electrode surfaces indicate that the cycle life
2015; Pavlov et al., 2012; Murali et al., 2017). of batteries with carbon lead hybrid electrodes
In addition, the lead crystals formed on the could be prolonged. Further experiments are
negative electrode with carbon cloth addition ongoing to demonstrate the newly designed
have a smaller size than those formed on the battery works effectively under different
negative electrode with carbon paper addition. working conditions, and will be published in the
This could be due to the higher flexibility of future.
carbon cloth than carbon paper, which provides
better contact between the carbon cloth and Acknowledgements
the negative electrode surface, leading to
better electron conduction during the chemical We are thankful to CeTech Co Ltd., Taiwan
reactions. This observation is consistent with for supplying carbon materials and Taiwan
the initial capacity results in which the better KUNG LONG batteries industrial CO., LTD for
providing lead-acid batteries.

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IMPROVING PERFORMANCE OF LEAD-ACID BATTERIES THROUGH CARBON LEAD 99

Figure 6: SEM images of negative electrode surface after discharge to 1.6 V: (a) without carbon material; (b)
with carbon paper; (c) with carbon cloth

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