Overview of Graphene as Promising Electrode materials for Li-ion

Battery
Md Sohanur Rahman1, Bapi Mondal2*, Md Masum Parvez2, Md. Mehedi Hasan2, Bushra Saba2,
Istiuqe Ahmed2, Aqib Adnan Shafin2, Md. Mahmud2
1
Department of Advanced Functional Materials, Technical University of Chemnitz, Germany
2
Department of Applied Chemistry and Chemical Engineering, Bangabandhu Sheikh Mujibur Rahman
Science and Technology University, Gopalganj, Bangladesh.
*
Corresponding author (email: [email protected])

Abstract.
The energy and storage sector of today's world is constantly facing challenges in terms of the
performance, functionality of the fundamental materials. Graphene is a Carbon-based material
that is extensively investigated as anode material for rechargeable secondary Lithium-ion
batteries (LIBs) because of its amazing superlative properties i.e. mechanical, optical, electrical,
thermal, and sensing properties. Graphene has extraordinary electron mobility (2.5×105 cm2 V-1 s-
1
) and a large surface area (2630 m 2g-1) and these interesting properties make it a suitable
material for the energy storage device. Also Nanostructure evolution of graphene, its
electrochemical performance raised to a new stage. In this review, we focus on the
electrochemical performance of graphene and Graphene-based nanocomposite materials in
Lithium-ion Batteries and also focuses on the synthesis route of graphene which is used both
industrially and commercially.

Keywords: Graphene, Lithium-ion Battery, Electrochemical Performance, Electrode materials.

1. Introduction
Lithium-ion batteries (LIBs) are widely used as energy storage devices with Compared to
other types of batteries due to their various types of major advantages together with high energy
density, high columbic, and energy efficiency, zero memory effect, comparatively long cycle
life, and edibility in modification, which make LIBs desirable for a wide range of products such
as smartphones, laptop computers batteries and mobile power banks.[26] The energy and storage
sector of today’s world is repeatedly facing provocation in terms of performance, functionality of
the fundamental materials.[38] To fulfill the demand for electrochemical energy storage,
especially for portable and the lightweight electronic devices, secondary lithium-ion batteries
were introduced into the global market for a long period of time. Sony for the first time
commercialized lithium-ion battery (LIB) in 1991. But also sodium-ion battery is opening the
possibilities of beginning its commercial journey as a swap of LIB.[27] [28]

A secondary lithium-ion battery or Li-ion battery (abbreviated as LIB) is mainly a reversible

battery, 1st outlined by chemist M Stanley Whittingham at Exxon within the Seventies. Lithium-
ion batteries are ordinarily used for moveable physics and electrical vehicles and are growing in
quality for military and regional applications. Lithium is the lightest of metals and it can easily
float on water. The electrochemical properties of lithium are exceptional and it is also a highly
reactive material. This characteristic gives Lithium the potential to achieve very high energy and
power densities in high-density battery utilization such as automotive and standby power. A
lithium cell can yield voltage from 1.5 V to 3 V depends on the types of materials used.[29] [30]

Lithium-ion batteries are gain enormous attention in terms of their marvel electrochemical
properties. The lithium-ion battery is rechargeable, lightweight, and comparatively low cost.
However, researchers are always finding a possible solution for reducing LIB cost and its weight
and size.[30][31]

1.1 Working Principle

Lithium-ion batteries are working on an interesting concept based on the electrochemical
potential associated with the metal. Electrochemical potential means the tendency to lose
electrons of a metal.
Now a general electrochemical potential series is shown below
Li Mg Al Zn Fe H Hg Cu Ag F

3.04V 2.37 V 1.66 V 0.76 V 0.44 V 0V -0.24V -0.34V -1.69V -2.8V

Potential in Voltage

12
10
8
Potential in Voltage (V)

6 0
0.44 Florine (F); 10
4 0.76 Copper Silver (Ag); 9
2.37 1.66
HydrogenMercury
(H); 6 (Hg); 7 (Cu); 8
2 3.04 Zinc3(Zn); Iron
4 (Fe); 5
Magnesium Aluminium
(Mg); 2 (Al);
0 Lithium(Li); 1 -0.24 -0.34 -1.69 -2.8
Lithium(Li)

Magnesium (Mg)

Aluminium (Al)

Zinc (Zn)

Iron (Fe)

Hydrogen (H)

Mercury (Hg)

Copper (Cu)

Silver (Ag)

Florine (F)

-2
-4

Name of Various Metal

Figure 1 Electrochemical Potential Series of Various metals.

According to these values, Li is the highest tendency to lose an electron. Li metal is lightweight.
Similarly, exposing a huge amount of charge storing capacity. Due to this reason, Li-ion battery
occupies a wide range of electronics sectors, power devices, electric vehicles automobile parts
engines, laptops, etc.
LIB batteries are two major working mechanisms one is the Discharging mechanism and the last
one is the charging mechanism which is illustrated by the following figure

Figure 2 Lithium-ion battery charging and discharging mechanism

While discharging Li-ions are detached from the anode and migrate across the electrolyte and are
inserted into the crystal structure of the host compound of the cathode. Again during charging,
lithium in positive electrode material is ionized and travels from layer to layer, and added into
the negative electrode. Ordinary lithium-ion batteries used graphite as an anode and lithium
metal oxide compound as a cathode. The overall cell reaction is mainly divided into two
categories as charging reaction and discharging reaction. The reaction is described below

During discharging
At anode: LixC→ xLi+ + xe- + C
At cathode: Li1-xMO2 + xLi+ + xe-→ LiMO2
During charging
At anode: xLi+ + xe- + C→ LixC
At cathode: LiMO2→ Li1-xMO2 + xLi+ + xe-

But when the battery is in over-discharge then Li2O is produced from LiCoO2
Li+ + e- +LiCoO2 → Li2O + CoO
Therefore in extreme overcharge CoO2 is produced.
LiCoO2 → Li+ + CoO2 + e-

1.2 Construction
The three initial structural components of a lithium-ion battery are the positive and
negative electrodes and electrolytes. Ordinarily, the negative electrode of a traditional lithium-
ion cell is manufactured from natural carbon. The positive electrode is a metal oxide, and the
electrolyte is a lithium salt in an organic solvent. The battery consists of an anode of Lithium,
diffuse as ions, into a carbon. The cathode material is made up of Lithium liberating compounds,
typically the three electro-active oxide materials such as Lithium Cobalt-oxide (LiCoO 2),
Lithium Manganese-oxide (LiMn2O4), and Lithium Nickel-oxide (LiNiO2).
Li-ion cell has a four-layer structure.
● A positive electrode material is known as an anode.

● A Negative electrode material is known as Cathode.

● A separator is a fine porous polymer film.

● An electrolyte made with lithium salt in an organic solvent. The electrolytes are selected
in such a way that there should be an effective transport of Li-ion to the cathode during
discharge.
However, in this review, we will concentrate only on the anode materials, and in the last section
of this review, we will demonstrate that Graphene is a promising anode material for secondary
lithium-ion batteries due to its amazing superlative properties.

1.3 Graphene-Based Anode in LIB

Carbon-based materials including carbon fiber, carbon nanotube (CNT), carbon
nanoribbons, graphite, graphene, etc. as battery electrode materials have advanced in this
research field toward the studious stage. By comparing with all the carbonaceous electrode
materials, graphene acquires the most potential to face the challenges of the power and storage
sectors.[33]

The marvel material graphene is literally one atom thick sheet of carbon organized in an SP 2-
bonded hexagonal framework. Further Graphene is a two-dimensional one-atom-thick planar
sheet of sp2 bonded carbon atoms, which is shown in Figure 2. In extension to its planar state
graphene can be categorized into 0D/1D/2D dimensional Graphene. Consequently, graphene can
be expressed as the mother of all carbon forms.[1]
 Figure 3 Mother of all Graphene forms. Graphene is a 2D building material for carbon material of all other
dimensionalities. It can be wrapped up into 0D Buckyballs, rolled into 1D nanotubes, or stacked into 3D graphite.
[2]

Nobel laureates Geim and Novoselov discover this marvel materials graphene and they show
numerous applications of graphene depending on its wide range of properties. Graphene exposes
many charming characteristics including mechanical, optical, electrical, thermal, and sensing
properties. Graphene has extraordinary electron (e-) mobility (2.5×105 cm2 V-1 s-1) and a large
surface area (2630 m2g-1) and these interesting properties make it a suitable material for energy
storage devices. The service and performance of graphene have been checked by researchers
around the world for versatile application along with its usages as an electrode (anode/cathode)
and electrolyte for secondary rechargeable batteries. Despite having such interesting potential,
the future of commercial-scale synthesis of graphene is now in a challenging stage. Production of
a large number of high-quality graphene productions is hope or challenge for the future. In this
review, our purpose is to inspect the growth of graphene-based electrode materials used in LIB.
[2]

2. Graphene Synthesis Route

Most of the Graphene is synthesized from Natural Graphite but this method is
unconventional and very difficult as well as costly. Many researchers and investigators produced
graphene by using many routes and some of them produce Graphene on large scale and
industrially. Now all the possible routes for the synthesis of Graphene are represented by the
following Hierarchy chart.
 Graphene Synthesis Route

Top Bottom
Down Up

Chemical
Mechanical Chemical Chemical Epitaxial
Pyrolysis Vapour Other
Exfoliation Exfoliation Synthesis Growth
Deposition

Adhesive Thermal Plasma

Reduction GO
Tapes Process Process

Figure 4 Routes for Graphene Synthesis.

Natural graphite is the main raw material for the extraction of graphene. For this reason, we do
not need to create graphene architecture, rather need to exfoliate it from graphite. Novoselov and
Geim are the first to exfoliate graphene back in 2004. They used the scotch tape method to peel a
layer of graphene from a highly ordered pyrolytic graphite sample. Still, this mechanical means
of graphene production yield a product of the highest quality but cannot be used commercially
because of the constraint of large-scale production.[3]

However, in this review, we will describe a few specific processes for Graphene synthesis
because these methods are very consistent and most available. Many researchers choose these
routes for the production of a large amount of Graphene. Graphenes are mainly conventional
natural graphite. Researchers choose Graphite as a raw material for the production of industrial
graphene. The top-down and bottom-up approach is the main synthesis methods which are
subdivided into many categories.[4]

2.1 Top-down Method

The top-down approach involves the exfoliation of graphene from a precursor material
mostly graphite. The mechanical method, chemical method, electrochemical method, etc. are
various top-down methods. Among them, the chemical method gained huge attention due to its
advantages of moderate quality and quantity production at low cost and ease in synthesis
procedures. Usually in this method, graphite is oxidized to produce graphene oxide (GO) by
chemical means and then subsequently reduced into graphene. This reduction can be done by
various techniques, i.e. thermal, chemical, solvothermal, photocatalytic, etc. In recent years,
several modifications have been done in other top-down approaches.[5]
 Figure 5 Top-down method for Graphene Synthesis.[5]

2.2 Bottom-up Method

Bottom-up approaches involve the growth of graphene on a precursor substrate. Chemical

vapor deposition (CVD), epitaxial growth on SiC, pyrolysis, etc. are the various bottom-up
approaches of graphene synthesis. Very high-quality graphene layers can be found by the
Chemical vapor deposition and epitaxial growth methods, and therefore, these two methods are
widely used in the laboratory for graphene research purposes.[6]

Figure 6 Bottom-up method for Graphene synthesis.[6]

2.3 Summarizations of Few Top-down and Bottom-up Synthesis methods.

Top-Down method

Dimensions
Name of Essential
Latera Advantages Disadvantage’s Ref
Methods Thickness Chemicals
l

Micromechanical Slight µm up Highly Broad size Low yields, [7,8]

exfoliation layers to cm ordered and High Costly
unmodified process.
pyrolytic
graphite graphene
(HOPG), sheets,
unique
crystal 2%
 absorption
graphite,
rate.

Single Unmodified
µm up graphene, A low quantity
Direct sonication and
to sub- Graphite of graphene [9]
of graphite Double Low costly
µm yields.
layers process.

Polymer
composites
Single-step
, Graphene
production
oxide
and
Electrochemical Single 500- (GO),
exfoliation High ionic
and slight 700 KMnO4, [10,11]
exfoliation yields high liquid cost.
layers nm and NaNO3
inH2SO4/ Electrical
conductive
H3PO4 as
graphene.
oxidizing
agents.

Bottom-Up method

Dimensions
Essential
Methods Latera Advantages Disadvantage’s Ref
Thickness Chemicals
l

High-
quality The larger
Small scale
Chemical vapor Slight Very graphite, size and
production, Not
large Transition high-quality [12]
Deposition(CVD) layers used
in cm metal graphene
commercially.
including produced.
Ni, Cu, Pd

Epitaxial growth Slight Up to Silicon Yields Very small [13]

on Silicon cm carbide graphene scale
Carbide (SiC) layers size (SiC) show a large production.
surface surface area.

Easily size
Unzipping of Multiple Carbon controlled by
Less Expensive
carbon nanotubes or double nanotube selection of [14]
µm process
(CN) layers (CNT)
CNT
 Table 1 Top-down and Bottom-up methods summary

3. Graphene as Anode in LIB

Investigator says that Graphene acts as promising electrode material in LIB as a result of
its some awesome appealing properties like high surface to volume ratio, ultra-thin thickness,
electrical conductivity, structural flexibility, etc. Similarly, these materials are very much needed
for use as an electrode in LIB. Liu et al. work on graphene and they demonstrate how to expand
the capacity of graphene.[15] They successfully integrated two Li atoms on the twin sides of
graphene single layer maintaining stoichiometry of Li2C6 having a specific capacity of 540
mAHg-1better than Li-intercalated graphite.[15] [33]
Bhardwaj et al. showed that the capacity increments of graphene in the year 2010. By using
carbon nanoribbons they successfully expand the Li-ion storage capacity. They extracted GNRs
by unzipping pristine multi-walled carbon nanotubes. The authors showed oxidized GNSs
outperformed in terms of energy density than all other materials tested (GNSs and MWCNTs).
Oxidized GNRs had the first charge capacity of ~1400 mAhg -1 with low columbic efficiency for
the first cycle (~53%) and reversible capacity in the range of 800 mAhg -1 [16][33-37]. Now
lithium-ion insertions and De-insertions of properties of various Graphene families are shown in
figure 7.

Figure 7 Charge and discharge properties of (a) Graphite (b) graphene nanosheet (c) GNS incorporated with
carbon nanotube[17]
 Capacity Range in (mAh/g)

Graphite 372

Graphene 540

GNS+CNT 730

GNS+C60 784
0 100 200 300 400 500 600 700 800 900

Capacity Range
Figure 8 Comparison of Capacity of Various Carbon-based electrode materials [18].

Summarizations of LIB Anode materials involving Graphene

Materials Synthesis Route Capacity and Cycle Performance Ref

SnO2/graphene Hydrothermal The preliminary discharge capacity of [19]

1588 mAh/g

After 40 cycle its remain 730 mAh/g

Si/graphene Hydrazine reduction/ The preliminary discharge capacity of [20]

chemical reductions 2753 mAh/g

After 50 cycle its remain 590 mAh/g

CuO/graphene N-methyl-2-pyrrolidone Preliminary discharge capacity 640mAh/g [21]

solvent
Later 50 cycle its remain 582 mAh/g

Fe3O4/graphene Graphene oxide (GO) The initial discharge capacity of 1426 [23]
reduction mAh/g

After 50 cycle its remain 1160 mAh/g

Table 2 Summary of LIB anode materials containing Graphene which is incorporated with some other non-carbon
metals.

4. Conclusion
Compared to old-fashioned carbon conductor materials, Graphene, because of its low
initial coulombic potency, high charge and discharge profile, and different shortcomings, cannot
directly alter pristine carbon as associate degree anode material on an extensive scale. After all,
Graphene will exhibit high electrical physical phenomenon, smart mechanical strength,
wonderful flexibility, nice chemical stability, and high specific expanse. Once used as conductor
material, Graphene will effectively cut back the scale of the active material, forestall
agglomeration of nanoparticles, and improve electrons and ions transmission capability,
additionally enhancing the electrode's mechanical stability. Firstly, graphene’s flexibility makes
it a perfect material to buffer the metal electrode's volume growth and contraction throughout the
charge-discharge method. Together with, Graphene exhibit higher lithium metal particle storage
capability and advanced cycle life to replace the traditional carbon. Furthermore, Graphene
retains its cycle life when several cycles than traditional graphite type anode materials.
Additionally, the investigator has taken numerous approaches to produce graphene on a massive
scale. When graphene is incorporated with other alloy-type materials such as silicon, tin, copper
oxide its electrochemical performance is enhanced greatly.
To bring this graphene-based anode into a commercial scenario as an upgraded version anode for
the future-generation rechargeable battery, researches in this area has reached a potential state.
Hopefully, it is not much when the effective application of graphene-based, as well as graphene-
based composite materials as an anode in rechargeable batteries, will be treated as a
breakthrough in battery performances.
Acknowledgment
These review articles are based on various journal articles, research papers, and also follow many
researchers' works on carbon-based graphene. The authors are grateful to all the participants of
this work.
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