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Application of Graphene in Lithium-Ion Batteries

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Chuanlei Qi, Jiaran Wang, Shengping Li, Yuting Cao, Yindong Liu and Luhai Wang

Submitted: 20 August 2023 Reviewed: 07 February 2024 Published: 06 March 2024

DOI: 10.5772/intechopen.114286

Graphene - Chemistry and Applications IntechOpen
Graphene - Chemistry and Applications Edited by Enos Wamalwa Wambu

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Graphene - Chemistry and Applications [Working Title]

Dr. Enos Wamalwa Wambu

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Abstract

Graphene has excellent conductivity, large specific surface area, high thermal conductivity, and sp2 hybridized carbon atomic plane. Because of these properties, graphene has shown great potential as a material for use in lithium-ion batteries (LIBs). One of its main advantages is its excellent electrical conductivity; graphene can be used as a conductive agent of electrode materials to improve the rate and cycle performance of batteries. It has a high surface area-to-volume ratio, which can increase the battery’s energy storage capacities as anode material, and it is highly flexible and can be used as a coating material on the electrodes of the battery to prevent the growth of lithium dendrites, which can cause short circuits and potentially lead to the battery catching fire or exploding. Furthermore, graphene oxide can be used as a binder material in the electrode to improve the mechanical stability and adhesion of the electrodes so as to increase the durability and lifespan of the battery. Overall, graphene has a lot of potential to improve the performance and safety of LIBs, making them a more reliable and efficient energy storage solution; the addition of graphene can greatly improve the performance of LIBs and enhance chemical stability, conductivity, capacity, and safety performance, and greatly enrich the application backgrounds of LIBs.

Keywords

  • conductivity
  • electrochemical processes
  • electrode materials
  • graphene oxide
  • graphene materials
  • lithium storage
  • lithium-ion batteries

1. Introduction

During the Industrial Revolution, the world rapidly developed and economically prospered with clean, affordable and reliable energy [1]. The consumption of traditional fossil energy has attracted widespread attention from various industries, and environmental protection has driven research on alternative energy supplies, especially renewable energy, and efforts are being made to develop new renewable energy types while providing an effective environmental protection approach [2, 3].

In order to meet the growing energy demand and reduce greenhouse gas emissions, many countries have recently conducted extensive research on low-cost and environmentally friendly renewable energy sources, such as solar, tidal, wind, biomass, and geothermal [4]. At the same time, it is necessary not only to develop energy but also to maximize energy storage. In addition, there has been a renewed interest in electric vehicles as substitutes for internal combustion engine vehicles, which account for 25% of greenhouse gas emissions [5], making energy storage a priority for the new global energy management system.

Electrochemical energy storage technology has obvious advantages among the various energy storage technologies. The battery is not limited by geographical location, convenient and efficient charging and discharging processes, and higher efficiency [6]. As the main force of energy storage technology, electrochemical energy storage has received widespread attention in market development and scientific research fields. At present, mainstream electrochemical energy storage technologies include LIBs [7], lead batteries [8], and flow batteries [9]. Among them, the LIBs have the characteristics of long cycle characteristics, fast response speed, and high system comprehensive efficiency and are widely used in portable charging equipment, transportation systems, aerospace, and other fields [10, 11].

However, the energy storage processes of the LIB electrode systems are different from each other. With the demand for reliable and durable energy storage devices in portable electronic products and power grids, improving the power density and cycle life of LIBs has become an important goal [12, 13]. It is crucial to design and manufacture efficient electrode materials that can provide high specific capacity and energy density to meet the growing demand for high-performance electrical equipment [10, 14].

Since the energy density of LIBs depends largely on electrode materials, the research direction is aimed at high-specific capacity electrode materials. It has been recognized that nanostructured electrode materials with special electrochemical properties will be necessary to achieve the purpose. The dimensionality reduction of nanomaterials can shorten the diffusion time of Li+ [15].

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2. Overview of the graphene chemistry

Graphene and carbon nanotubes [16] have played important roles in nanomaterials, which can be applied to portable communication equipment, electric vehicles, and large-scale energy storage systems. Many research results have shown that energy storage technology could achieve a qualitative leap by breaking through the technical difficulty of electrode nanomaterials named graphene, a novel two-dimensional carbon material that was discovered by mechanical exfoliation of graphite in 2004 [17]. As illustrated in Figure 1, the typical structure of graphene [18] is composed of a carbon material 1 million times thicker than the diameter of a single hair comprising a hexagonal two-dimensional honeycomb lattice of sp2 hybridized carbon atoms. The structure can be divided into single-layer, double-layer, and multilayer, with an ultra-high specific surface area of about 2630 m2 g−1.

Figure 1.

(a) and (b) Typical structure of graphene [18].

Graphene has many desirable properties, with very high electron mobility at room temperature and rapid heterogeneous electron transfer at the edges, with values exceeding 15,000 cm2 V−1S−1 [19]. Graphene also has a significantly high Young’s modulus (1.0 TPa), high breaking strength, extraordinary mechanical strength, excellent thermodynamic, electrical conductivity (5–6.4 × 106 S m−1), optical transmittance activity (about 97.7%), material density (less than 1 g cm−3), stability, catalytic properties, and other graphene tunable properties [20, 21].

The continuous two-dimensional conductive network formed by graphene can effectively improve the electron and ion transport kinetics of electrode materials, and graphene is used to improve the rate performance and cycle stability of LIBs because of its high specific surface area, stable chemical properties, excellent electrical and thermal conductivity [18]. With its excellent characteristics, graphene has lots of applications in electronic devices, photonic devices, photocatalysis, and advanced composite materials applicable in the military, aerospace, and other fields.

Although graphene shows excellent properties in chemical and mechanical aspects, its application in electronics and energy storage devices needs to be continuously explored [22]. Researchers have developed many methods in graphene applications, such as combining with other materials to develop graphene-based composites [23] including graphene/polymers [24], graphene/metals [25], and graphene/carbon nanotubes [26] composites for energy storage devices.

In addition, recent scientific advancements have allowed the development of various low-cost and environmentally friendly methods for preparing graphene. This is particularly important for large-scale production and application. The following analysis analyzes the application of graphene and graphene-based nanocomposites as electrode materials in LIBs, and provides possible development paths in the future.

The main production methods for graphene include bottom-up and top-down methods, and graphene properties have great differences in structural integrity, sheet size, and cost with different methods [27, 28]. As illustrated in Figure 2, the top-down approach refers to the method of obtaining a product by crushing or peeling off a large amount of material. The bottom-up approach, on the other hand, refers to the method of synthesizing the desired product from smaller materials, continuously growing graphene by breaking the chemical bonds of carbon-containing compounds and depositing carbon atoms on a suitable substrate [29, 30, 31, 32]. Various forms of graphene nanomaterials have been prepared, including graphene spheres, graphene scrolls, graphene networks, graphene tubes, graphene cages, and other structures of graphene [21].

Figure 2.

(a) Schematic diagram of top-down and bottom-up approaches, (b) schematic diagram of graphite structure [29].

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3. Lithium-ion batteries, LIBs

As shown in Figure 3, lithium-ion batteries (LIBs) consist of two electrodes and a separator impregnated with an electrolyte to provide the electrons and ions needed for electrochemically active nanomaterials [33].

Figure 3.

Schematic diagram of the structure of commercial LIBs [33].

The metal-foil anode is the negative electrode of the battery, and it is made of lithium-containing material. During discharge, lithium ions are released from the anode and travel through the electrolyte to the cathode, where they are intercalated (inserted) into the electrode material. The anode also serves as the current collector for the negative terminal of the battery. The cathode, or positive electrode, is made of an electron-rich material that can store the lithium ions after they are released from the anode. It is typically coated onto a metal foil current collector. During discharge, electrons flow through the external circuit to the cathode, where they combine with the lithium ions to form the discharge product. The separator is a thin film that separates the anode and cathode to prevent direct contact between them. It is made of a material that is permeable to lithium ions but impermeable to electrons, ensuring that the electrons flow through the external circuit during discharge and charge. The separator also helps to prevent short circuits within the battery. The electrolyte is a liquid or solid material that transports the lithium ions between the anode and cathode. It is typically a lithium salt dissolved in a non-aqueous solvent.

The LIBs are based on the movement of lithium ions between the anode and cathode during discharge and charge cycles. When the battery is discharged, electrons flow through the external circuit to the cathode, where they combine with lithium ions to form the discharge product. At the same time, lithium ions travel through the electrolyte.

At the moment, LIBs are regarded as one of the most promising energy storage technologies due to their high energy density, energy conversion efficiency, and output voltage [34]. With the development of information electronics, electric vehicles, and smart grids, there is a huge demand for LIBs with high energy density, long cycle life, and lower cost [35, 36]. However, the electrode materials of LIBs generally have poor conductivity, and the charge-discharge reaction cannot be completely carried out due to electrode polarization during the charging and discharging process. Moreover, the effective capacity of the electrode material cannot be fully exerted [37, 38, 39].

At present, the conductive agents on the market mainly include conductive carbon black, conductive graphite, and carbon nanotubes [40]. The excellent thermal conductivity of graphene can improve the thermal stability of LIBs. The “face” contact between graphene and electrode materials can improve the conductivity of electrodes [41]. Based on the special physical and chemical properties of graphene, and it has great potential as an electrode material for LIBs. LIBs are composed of four parts: cathode electrode material, anode electrode material, separator, and electrolyte, and the electrode material plays an important role in battery performance [42, 43]. According to application fields, the application of graphene mainly has three directions in LIBs: (1) graphene use as an active electrode material: graphene can be used as an anode material for LIBs to provide reversible storage space for Li+, improving specific capacity and rapid charge and discharge efficiency [44]. (2) Graphene can be combined with cathode or anode materials to improve the performance of electrodes: the combination of graphene with a cathode active material enhances electrode conductivity [45]. In this respect, graphene can be compounded with anode-active materials to construct a three-dimensional structure and provide space for volume expansion [46]. (3) Graphene is used as a conductive additive to provide a fast channel for electron and Li+ transport and improve the conductivity of the electrode [47, 48].

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4. Graphene as LIBs electrode conductive agent

At present, the development of energy storage technology has made higher requirements for LIBs in terms of energy density, ion transport rate, and cycle performance [49]. However, the poor conductivity of electrode materials greatly limits the performance of LIBs. Adding a conductive agent can enhance the electron transport efficiency and reduce the polarization of the electrode. It is important to utilize the effective capacity of the active material. Compared with conductive agents such as commercial conductive agent carbon black (CB), graphene has higher conductivity and specific surface area, and studies have shown that advanced carbon materials, including carbon (one-dimensional) [50], graphene (two-dimensional) [51, 52], and 3D graphene backbones (three-dimensional) [53], have been used to build continuous conductive networks for LIBs [54].

Graphene is a powerful planar conductive additive, which is considered to be one of the most promising conductive additives due to its unique physicochemical properties including high aspect ratio, chemical resistance, excellent conductivity, and low dosage of effective characteristics [55, 56, 57]. Compared with the “point-to-point” contact mode constructed by the traditional graphite conductive agent, graphene can form a “point-to-surface” contact mode with the electrode material in the electrode, providing a long-range and fast conduction path for electrons and Li+, reducing the amount of conductive agent is equivalent to increasing the content of the active material of the electrode and increasing the capacity of the electrode [54, 58]. Therefore, using a small amount of graphene as a conductive additive can greatly improve the electronic conductivity of the electrode.

It has been proposed as a simple and effective method to prepare graphene conductive slurry as a conductive agent for LIBs by combining mechanical stirring, ultrasonic dispersion, and dispersant modification [48]. Figure 4a shows the schematic diagram of graphene dispersion. Graphene slurry also exhibits excellent battery performance as a conductive agent for LIBs. At 100 mAg−1 current density, the first charge and discharge capacity are 1273.8 and 1723.7 mAhg−1, respectively, and the coulombic efficiency is 73.9%. The capacity retention rate of the anode is 84% (1070.2 mAhg−1) after 100 cycles at 200 mAg−1. Another article reported that graphene nanosheets (GN) with different sizes as conductive additives can affect the electrochemical performance of LiFePO4 (LFP) [61]. Compared with conventional conductive additives, GNs and Super P Conductive Carbon Black (SP) can construct an effective electronic conductive network and significantly improve the electrochemical performance of LFP as conductive additives. It also shows that with the increase of GN size, the specific capacity and rate performance of nanoscale LFP tended to deteriorate, which is due to the “barrier effect” of GN extending the length of the ion transport path and greatly reducing the ion conductivity. The small-size GN can effectively balance the rapid diffusion of Li+ and the electron transport of nanoscale LFP. The effect of the amount of graphene used in different thicknesses electrode on the electrode performance was also studied [59]. The results showed that when the thickness of the electrode is thin, the cycle performance and rate performance of the electrode increase with the increase of graphene addition (Figure 4b). When the electrode thickness is higher, the rate performance of the electrode has a linear relationship with the amount of graphene. The Li+ diffusion path is greatly extended, and the spatial effect of GN is amplified, causing slower ion transport kinetics. Different research results indicate that the conductivity of the electrode material is significantly improved when the amount of graphene is appropriate. However, when the size or the amount of the graphene nanosheet (GN) is too large in the higher-thickness electrode, the Li+ diffusion path will be greatly extended. The steric hindrance effect of graphene on the diffusion of Li+ is amplified, the polarizability is higher at high rates, and the rate of performance of the electrode is reduced. So, researchers should pay attention to maintaining the balance between ion diffusion kinetics and electron conduction when using graphene as a conductive agent.

Figure 4.

(a) Schematic diagram of graphene dispersion, (b) schematic diagram of the evolution of electrode thickness from laboratory half-coin battery to commercial soft-packaged battery [59], and (c) schematic diagram of lithium-ion transport path in LiFePO4 cathode with GN or HG + SP as conductive additive [60].

In order to improve the conductivity and the rate performance of LIBs, researchers have studied a lot on graphene composite conductive agents and graphene modification. Graphene nanoribbons (GNBs) have been used as a conductive agent for LFP [62]. The cathode with olivine structures is used to promote rapid redox reactions and achieve high-rate cell performance. The results have shown that the cathodes with 5 wt% graphene nanoribbons and 10 wt% conductive carbon nanoparticles exhibited a capacity of 163.25 mAhg−1 at 0.1 C and 130.60 mAhg−1 at 2 C, the capacity retention rate is 98.21% after 100 cycles at 2 C. Graphene nanoribbons play the role of bridges creating connected networks to facilitate electron transport. Porous graphene (HG) has been prepared by KOH activation [60]. HG, with a large number of pores and a large specific surface area, greatly improved the electronic conductivity of the LFP electrode, but it did not affect the efficient transport of ions. LFP cells with traditional graphene additives exhibit lower rate performance because graphene with a planar structure hinders the transport of Li+. Binary conductive additives containing only 1 wt% HG and 1 wt% carbon black (such as SP) can make LIBs obtain higher rate performance comparable to batteries containing 10 wt% SP, and the schematic diagram of the Li+ transport path of the composite conductive agent is shown in Figure 4c. A small amount of SP complements the remote conductive network formed by HG, which can fully contact LFP so that the entire LFP electrode has excellent conductivity. The simultaneous use of HG and SP can achieve a balance of electron conductivity and ion diffusivity.

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5. Application of graphene as LIBs cathode materials

As the cathode of LIBs, the electrode material should have the requirements of high reversible capacity, high stability potential, and lower manufacturing cost [63, 64]. At present, the cathode materials of LIBs are mostly LiFePO4, LiCoO2, LiMn2O4, Li3V2(PO4)3, and LiNixCoyM1-x-yO2, which have the characteristics of high specific capacity, non-toxicity, and low cost, but the conductivity is poor, and the mobility of lithium-ion is low [65, 66, 67].

When LiFePO4 material is compounded with graphene, theoretically, the rate performance can be improved as conductivity improves [68, 69]. The LPF-graphene composite, LFP@C/G, was successfully synthesized, as illustrated in Figure 5, using the high energy ball milling-assisted rheological phase method [70]. The multilayer graphene film is not stacked on the carbon-coated LiFePO4 nanospheres, thus forming rich mesopores forming unique 3D “ball-in-chip” and “ball-on-chip” conductive network structures. High conductivity and rich mesopores facilitate the transport of electrons and ions. The results show that the mixed materials with graphene content of about 3 wt% show excellent rate performance, and the initial discharge capacities were 163.8 and 147.1 mAhg−1, respectively. In addition, the composites also showed excellent cycling stability, with a capacity decay of only 8% after 500 cycles at 10 C. However, there are also reports that graphene composite LiFePO4 exhibits unfavorable electrochemical performance when used in cathode materials of LIBs. The effect of carbon coating on the electrochemical performance of LiFePO4 has been discussed [71]. The schematic diagram of the synthesis of lFP@graphene nanosheets (LFP@GN), sucrose-derived amorphous carbon-coated LFP (LFP@TC), and LFP/GN (partial wrapping) is shown in Figure 6a. Graphene partially wrapped LiFePO4 enhances the conductivity of LFP/GN material, but when the cathode material (LFP/GN) is fully wrapped in graphene, the ion transport efficiency decreases, leading to a decline in rate performance (Figure 6b). The results show that although graphene coating improved the conductivity of Li+ and electrons, the complete and dense coating of high graphitic carbon is not conducive to the transport of electrons due to the influence of steric hindrance effect on Li+ diffusion in the cathode material. Therefore, the ideal coating structure should maintain a balance between increased electron transport and rapid ion diffusion.

Figure 5.

Schematic diagram of the synthesis of LFP@C/G composites [70].

Figure 6.

(a) Preparation and electrochemical reaction protocols of LFP@TC and LFP/GN, (b) rates data of LFP@TC and FP/GN [66].

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6. Application of graphene as LIBs anode materials

As the most widely used anode material for LIBs, graphite anode has the advantages of easy access to abundant raw materials and low costs, but its low specific capacity falls short of meeting the requirements of LIBs [72, 73, 74]. The lithium dendrite formed during the charging and discharging process of graphite anode makes it difficult for LIBs to achieve high rate and cycle life [75], in addition to the fact that they can cause short circuits and potentially lead to the battery catching fire or exploding. Therefore, many studies are devoted to the modification of graphite anodes and the development of new anode materials.

At present, the typical lithium-ion battery anode materials can be divided into three categories: intercalation reaction electrode materials, conversion reaction electrode materials, and alloy electrode materials. The intercalated electrode materials are mainly composed of carbon materials [76]. There are many studies on the application of carbon materials in LIBs, and the research on graphene application in anode materials is more extensive and in-depth than in cathode. Graphene can react with Li+ on both sides of the graphene nanosheet to form LiC3, and each C atom corresponds to about 0.33 Li+, which is twice the amount of lithium intercalation in the traditional graphite electrode with a theoretical specific capacity of 744 mAhg−1 [77, 78]. Porous graphene foam (GF) has been prepared and applied as the anode of lithium-ion batteries. It comprises a loosely porous three-dimensional network structure with excellent electrical conductivity and chemical stability. GF has high performance in specific capacity and cycle stability. However, graphene as the anode material for LIBs may cause stacking between graphene sheets, reducing the specific surface area of the material, resulting in a decrease in lithium storage and failure to achieve higher capacity as a single anode material.

The graphene-metal composite material produced by the graphene coating method can, however, improve the electrochemical performance of LIBs [79]. The flexible characteristics of graphene can effectively inhibit the metal electrode volume expansion during the charging and discharging process, and the morphology of graphene can change with changes in the preparation method [52, 80, 81]. With excellent electrical conductivity, graphene can establish a conductive network between particles, and the high specific surface area can also increase the storage capacity of lithium. Numerous studies have shown that the graphene-metal composite materials applied as anode materials can greatly improve the performance of LIBs [52, 80, 81, 82]. The bilayer graphene (BGra) was synthesized by the thermal evaporation-deposition assisted chemical vapor deposition (CVD) method by coating on Si nanoparticles [83], as shown in the process diagram in Figure 7a–c. The results showed that the electrode composed of this material, Si@BGra, can provide a capacity of 2500 mAhg−1 at the current density of 3 Ag−1. At the same time, the capacity retention rate was 85% after 1000 cycles, exhibiting excellent cyclic stability (Figure 7d–f). The graphene-MnO2 composite was also prepared as anode materials for LIBs [84]. The material also demonstrated excellent cycle stability at current rates of 2 C, 5 C, and 10 C after 500 charge-discharge tests.

Figure 7.

(a) Schematic diagram of the preparation process of Si@BGra and Si@BGra/Ni (yellow represents silicon nanoparticles, orange is copper powder, gray is double-layer graphene, green is nickel foam), (b) SEM image of Si@BGra/Ni, (c) HRTEM image of Si@BGra/Ni, (d) Si@BGra/Ni magnification performance image at 1.0-50 Ag−1, (e) Si@BGra/Ni cycle performance at 20 Ag−1, and (f) cycling performance of Si@BGra/Ni at 3, 5, and 7 Ag−1 [83].

The excellent cycle stability and higher rate performance of these composites can be attributed to the integration of graphene and mesoporous metallic material. Graphene, as an exceptional charge carrier, enhances the electronic conductivity of composite materials and enables complete reversible redox reactions in metallic materials. As in LIBs anode materials, graphene can also act as a buffer medium for large volume changes of the negative electrode material during the charging and discharging process and inhibit mechanical strain and the crushing of electrodes.

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7. Application of other graphene derivatives in LIBs

Although graphene exhibits excellent electrochemical performance in electron and ion transport kinetics, its hydrophobic properties are challenging in electrode applications. As a strong and flexible carbon atom thin film, graphene offers a variety of possibilities for the modification and functionalization of its carbon backbone, such as chemical modification of H and O functional groups, so that its hydrophilic version of oxygen/hydrogen functionalization has recently gained popularity [85, 86, 87]. At present, the doping of heteroatoms into graphene to produce more Li+ storage sites has been widely studied. Heteroatom doping produces a large number of defects on the graphene surface, which not only prevents the irreversible aggregation of the graphene layer but also provides a rich lithium reservoir [86]. At the same time, the surface of graphene derivatives such as graphene oxide (GO), nitrate graphene, and fluorographene, has a large number of functional groups, defects, and other active sites, which enhance the electronic and mechanical properties of graphene [88].

Graphene oxide is usually prepared by stripping of graphite oxide generated by chemical oxidation, and the use of strong oxidants to generate graphite oxide is the most common method for preparing graphene oxide [89]. At present, the production of GO and reduced graphene (r-GO) have been commercialized. They form the basic units for forming other 3D graphene complex material, which also has the problem of low relative conductivity [90, 91]. High-quality foamed graphene and vertical graphene prepared by chemical vapor deposition (CVD) and plasma-enhanced chemical vapor deposition (PECVD) have emerged in the latest report, but the preparation process involves high temperatures and complex techniques. It is inferred that high-end 3D graphene derivatives with few defects and high electronic conductivity are the development direction in the future [92, 93].

Many researchers have devoted themselves to the study of graphene derivatives as lithium-ion cathode materials. A series of reduced porous graphene oxide (rhG-x) has been synthesized by the chemical oxidation and annealing reduction process of porous waste graphite (hSG) [94], and the schematic diagram of the process is shown in Figure 8. Because of the unique oxygen-containing groups and electronic conductivity, the rhG-x series with “worm-like” segments and porous structure diagrams shows excellent lithium storage performance as the cathode for LIBs.

Figure 8.

Schematic diagram of rhG-x synthesis process [94].

Few-layer graphene (FLG) has been prepared by a simple method to modify FLG using nitrogen doping. With the doping of heteroatoms, the rate performance and cycle stability of graphene were significantly improved [95].

In addition, graphene-based compounds are also widely used in LIBs. Uniformly dispersed Cu-hexahydroxytriphenyl (HHTP)/graphene (G) composites were synthesized using an in-situ growth strategy, and electrochemical performance was studied for the first time as anode for LIBs [96]. It was observed that graphene formed a two-dimensional network of conductivity in the composites and effectively improved the energy storage of Cu-HHTP.

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8. Application of graphene in thermal management of LIBs

Lithium-ion batteries have a wide range of applications in mobile communications, automobiles, and aerospace. With the rise of electric and hybrid electric vehicles (HEVs), there is another push for battery technology [97]. The battery and its management system are two of the three main technologies of electric vehicles, and the thermal management technology of the battery is an important part of the battery system. The operation life and efficiency of batteries are affected by high temperatures during working, thereby affecting the maintenance, life, and cost of electric vehicles [98, 99, 100]. Extending battery life and safe use of batteries requires controlling the operating temperature of LIBs within a safe range, and high or low temperatures will create adverse effects on LIBs. In addition, the electrolyte could solidify and fail to transport electrons at a lower temperature. Thus, the LIBs could experience thermal runaway or battery rupture or even explosion at high temperatures.

Many studies have shown that high, low, or uneven temperatures affect the charge-discharge efficiency and cycle stability of the power battery [101, 102, 103]. Therefore, it is necessary to design a reasonable battery thermal management system to effectively control and maintain a stable and uniform temperature of the battery in the battery pack. At present, the cooling methods of lithium-ion battery thermal management systems are mainly divided into three cooling methods: air cooling, liquid cooling, and phase change material (PCM) [104, 105].

A common method of thermal management of lithium-ion battery packs is based on the utilization of phase change materials (PCM) [106]. Phase change materials are a special class of functional materials that, in the phase change process, keep a small temperature change range or constant temperature and can absorb or release a large amount of latent heat [107, 108]. During the technological development of PCMs, researchers have studied many different kinds of materials, including inorganic systems (salts and salt hydrates), organic compounds (such as paraffins or fatty acids), and polymeric materials (such as polyethylene glycol) [109]. Paraffin wax is widely used as a phase change material in LIBs due to its excellent characteristics such as safety and non-toxicity, low price, small volume change during phase change, stable chemical properties, and low vapor pressure [110, 111]. However, there are some non-negligible shortcomings in the use of paraffin, such as easy leakage and low thermal conductivity during use of paraffin. Some materials with high thermal conductivity are usually combined with paraffin wax to improve their thermal conductivity and performance as PCM [112, 113, 114], considering the defect of low thermal conductivity of paraffin.

Researchers have combined some carbon materials with paraffin wax while using it in the thermal management of LIBs, and graphene is widely used due to its excellent thermal conductivity [115]. Graphene-epcm hybrid composites have been prepared by dispersing liquid phase stripping (LPE) graphene and FLG solutions in paraffin [116], and mixing them with high shear with a magnetic stirrer on a hot plate at 70°C. It is proved that graphene and FLG as fillers in organic phase change materials can improve their thermal conductivity by more than two orders of magnitude while maintaining their latent heat storage capacity. Graphene-coated nickel foam was prepared using chemical vapor deposition technology, and paraffin wax was used as a phase change material to penetrate into the voids of graphene-coated nickel foam. The thermal characteristics of saturated paraffin graphene-coated nickel foam and its application in the thermal management of LIBs were studied [117]. The results showed that: (1) the thermal conductivity of graphene @Ni/saturated paraffin wax was increased by 23 times compared with pure paraffin; (2) the melting temperature and freezing temperature of graphene-coated nickel foam composites of nickel foam/saturated paraffin were higher than paraffin wax and lower than paraffin, respectively.

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9. Conclusions and perspectives

In conclusion, the application of graphene in lithium-ion batteries has shown significant potential in improving battery performance. Graphene’s exceptional electrical conductivity, high specific surface area, and excellent mechanical properties make it an ideal candidate for enhancing the capabilities of these batteries. The various approaches, graphene derivatives, and graphene-based electrodes have been successfully utilized to improve the capacity, rate capability, cycling stability, and thermal stability of lithium-ion batteries.

However, there are still challenges that need to be addressed for the widespread application of graphene in lithium-ion batteries. One of the main challenges is the production of high-quality graphene in a scalable manner. The development of efficient and cost-effective methods for the synthesis of graphene is crucial for its commercialization in battery applications. Additionally, understanding the mechanisms behind the electrochemical performance of graphene-based electrodes is crucial for optimizing their properties.

Future perspectives in this field include exploring new applications of graphene beyond electrodes, such as in separators, electrolytes, and other battery components. The combination of graphene with other materials, such as metal oxides, carbon nanotubes, or polymers, may lead to the development of novel electrode architectures with improved performance. Furthermore, the development of 3D-printed graphene composites for battery applications is a promising direction that could lead to the production of customized battery components with improved mechanical properties and conductivity.

Overall, the application of graphene in lithium-ion batteries holds great promise for the development of next-generation energy storage devices with higher energy density, longer cycle life, and better rate capability. Continuing research efforts in this field are expected to lead to further advancements in the field of energy storage and pave the way for a sustainable future.

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Chuanlei Qi, Jiaran Wang, Shengping Li, Yuting Cao, Yindong Liu and Luhai Wang

Submitted: 20 August 2023 Reviewed: 07 February 2024 Published: 06 March 2024

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