Recycling of Graphite Anode FR

Received: 8 November 2022 Revised: 18 December 2022 Accepted: 28 December 2022
DOI: 10.1002/eom2.12321
REVIEW
Recycling of graphite anode from spent lithium-ion

batteries: Advances and perspectives
Yu Qiao 1,2 | Huaping Zhao 2 | Yonglong Shen 3 | Liqiang Li 4 |

Zhonghao Rao 1 | Guosheng Shao 3 | Yong Lei 2
1
School of Energy and Environmental Engineering, Hebei Key Laboratory of Thermal Science and Energy Clean Utilization, Hebei University of
Technology, Tianjin, China
2
Fachgebiet Angewandte Nanophysik, Institut für Physik & IMN MacroNano, Technische Universität Ilmenau, Ilmenau, Germany
3
School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, China
4
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, Institute of Molecular Aggregation Science, Tianjin
University, Tianjin, China
Correspondence
Zhonghao Rao, School of Energy and Abstract
Environmental Engineering, Hebei Key There is growing production for lithium-ion batteries (LIBs) to satisfy the
Laboratory of Thermal Science and
booming development renewable energy storage systems. Meanwhile, amounts
Energy Clean Utilization, Hebei
University of Technology, Tianjin 300401, of spent LIBs have been generated and will become more soon. Therefore, the
China proper disposal of these spent LIBs is of significant importance. Graphite is the
Email: [email protected]
dominant anode in most commercial LIBs. This review specifically focuses on
Guosheng Shao, School of Materials
the recent advances in the recycling of graphite anode (GA) from spent LIBs. It
Science and Engineering, Zhengzhou
University, Zhengzhou 450001, China. covers the significance of GA recycling from spent LIBs, the introduction of
Email: [email protected] the GA aging mechanisms in LIBs, the summary of the developed GA recovery
Yong Lei, Fachgebiet Angewandte strategies, and the highlight of reclaimed GA for potential applications. In
Nanophysik, Institut für Physik & IMN
MacroNano, Technische Universität
addition, the prospect related to the future challenges of GA recycling is given
Ilmenau, 98693 Ilmenau, Germany. at the end. It is expected that this review will provide practical guidance for
Email: [email protected] researchers engaged in the field of spent LIBs recycling.
Funding information
KEYWORDS
Chinesisch-Deutsche Zentrum für
Wissenschaftsförderung, Grant/Award graphite anode, recycling, regeneration, reutilization, spent lithium-ion batteries
Number: GZ1579; Deutsche
Forschungsgemeinschaft, Grant/Award
Number: LE 2249/15-1; Research
Foundation; Sino-German Center for
Research Promotion; China Scholarship
Council, Grant/Award Number:
202006420028
This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided
the original work is properly cited.
© 2023 The Authors. EcoMat published by The Hong Kong Polytechnic University and John Wiley & Sons Australia, Ltd.
EcoMat. 2023;5:e12321. wileyonlinelibrary.com/journal/ecomat 1 of 27

https://doi.org/10.1002/eom2.12321
2 of 27 QIAO ET AL.
1 | INTRODUCTION points of view, there is of great significance to recycle

spent LIBs.23–29 Particularly, recycling the valued compo-
Attributing to the advantages of high energy density, low nents (i.e., cathode, anode, and current collectors) in
self-discharge, and memoryless effect, lithium-ion batte- spent LIBs is an efficient strategy to address the challenge
ries (LIBs) have become the most promising secondary of resource scarcity.30 Meanwhile, it can effectively
batteries,1–5 and have been widely employed as energy reduce environmental destruction due to the excessive
storage units in portable electronics, electric vehicles, exploitation of resources.
aerospace applications, and large-scale electric energy At present, well-established hydrometallurgy,31
storage systems (Figure 1A).6–13 It is predicted that the pyrometallurgy,32 and bioleaching33 technologies have
global LIBs demand will approach up to 3600 GWh by been successfully employed in industrial production to
2030 (Figure 1B).14 However, limited by a certain service recover valuable metals from cathode materials in spent
life (3–10 years), amounts of spent LIBs have been gener- LIBs. In contrast, the efficient recycling of graphite anode
ated.15 Only in 2020, the global production of spent LIBs (GA) from spent LIBs is also economically and environ-
has exceeded to 150 000 tons,16 and will hit 3.7 million mentally important,34 but the progress lags behind cath-
tons by 2030 (Figure 1C).17 It is well known that LIBs are ode recycling. At present, GA occupies a dominant
mainly composed of four parts, for example, cathode, position in the anode market of LIBs,35 other anode
anode, electrolyte, and separator (Figure 1D).18 Cathode materials such as silicon-based anode, amorphous carbon
materials (such as LiCoO2, LiMn2O4, and LiFePO4) and and lithium titanate only account for about 9%.36 More-
anode materials (lithium titanate, silicon based compos- over, it is a little-known fact that 1 kg of graphite is
ites and graphite) are coated on aluminum foil and cop- needed for achieving 1 kWh of battery capacity of com-
per foil, respectively.19–21 The electrolyte is generally mercial LIBs, which means that the demand for GA in
made of lithium salts dissolved in high-purity organic sol- commercial LIBs is about 10–20 times higher than that
vents, while the separator is polyolefin-based porous for lithium.37 Considering the 12–21 wt% content of GA
membranes.22 From both economic and environmental in LIBs and the ever-increasing amount of spent LIBs,
F I G U R E 1 (A) Application fields of lithium-ion batteries (LIBs). (B) Estimated global battery demand by 2030. (C) Estimated global
spent LIBs market. (D) Schematic structure of LIBs
QIAO ET AL. 3 of 27
the disposal of GA from spent LIBs has attracted more and the commercial prospects of GA recycling are also
and more attention.38 On the one hand, the discard of prospected by reviewing the existing studies.
the spent GA will cause serious environmental pollution
because of the presence of undesired metal impurities
(including Li, Al, Co, Cu, Ni, Fe, and Mn)39 and toxic 2 | F A IL U R E ME C H A N I S M S A N D
organic electrolytes.40 On the other hand, all grades of CHARACTERISTICS OF GA IN
natural and synthetic graphite cannot be directly applied SPENT L IBS
to LIBs, and the production of battery-grade graphite is a
complex process. Natural graphite is mainly found in 2.1 | Failure mechanisms
associated graphite deposits, and its production mainly
including four steps: mining, beneficiation, purification The failure of LIBs refers to the attenuation or abnormal
and processing.41 Natural graphite mining not only has a performance of the battery caused by some specific rea-
huge impact on the environment (vegetation, air, water sons.44 It mainly divided into two categories: perfor-
pollution, etc.) but also poses a huge health risk (pneu- mance failure45 and safety failure.46 Performance failure
moconiosis) to the workers involved. To meet the represents the performance of LIBs fails to meet the ser-
requirements of battery grade graphite, it also needs to be vice requirements and relevant indicators, mainly includ-
treated with acid leaching, alkali roasting or inert ing capacity diving, attenuation of cycle life, abnormal
atmosphere heating treatment, which is also contrary to voltage, excessive internal resistance, self-discharge,
the requirements of clean production. Synthetic graphite high/low temperature failure, poor rate performance and
is made by calcining petroleum coke, needle coke and consistency. Safety failure refers to the failure of LIBs
bitumen at a certain temperature, then crushing, grading with certain safety risks due to improper use or abuse,
and high-temperature graphitization treating (usually mainly including thermal runaway, short circuit,
2500 C).42 High-temperature treating is supported by fos- gas/liquid leakage, lithium plating, expansion deforma-
sil fuels and electricity consumption, which result in tion, extrusion puncture and so on.47–50 In the view of
huge carbon emissions. It is proved that the energy micro-level, it can be investigated by internal causes and
consumption and greenhouse gas emissions in the the research scale can be traced back to the atomic and
graphitization stage are about 13.8 kg CO2-eq/kg and molecular scale. In addition, there are also some thermo-
45.9 MJ/kg, respectively.43 Currently, the price of dynamic and kinetic changes on the failure process.51
battery-grade graphite has reached as high as $8000– The failure occurs on anode materials usually including
$13 000/ton, accounting for nearly 10% of the overall solid electrolyte interface (SEI) overgrowth and decompo-
cost of LIBs.37 sition, lithium dendritic growth, particle breakage as well
In comparison, GA recovery from spent LIBs and its as current collector erosion.52,53 In the cases of both per-
further reuse in new LIBs would be more cost-effective formance failure and safety failure, the GA in LIBs will
and sustainable. Not only the reemployment as the anode be simultaneously destroyed due to (1) SEI decomposi-
in LIBs, but recovered graphite also possesses great appli- tion, (2) lithium dendrite and dead lithium, (3) graphite
cation potentials in the fields of supercapacitors, cataly- cracking and exfoliation, and (4) copper corrosion and
sis, and water treatment. Meanwhile, graphite recycling cracking, as shown in Figure 2. Next, the main failure
from spent LIBs will also be beneficial to environmental mechanisms occurs on GA are detailed discussed sepa-
protection. Given that, graphite recycling from spend rately, providing a theoretical basis for the structural
LIBs has gained more attention in the last years. changes in spent graphite.
In this study, we firstly start from the failure mecha-
nism of GA to provide a solid theoretical basis for under-
standing the structural changes of negative graphite. 2.1.1 | SEI failure
Next, the morphological and structural changes of spent
GA generated in the actual process were summarized, During the initial lithiation, an ionically conducting but
which provides important data support and directional electronically insulating SEI layer is firstly formed on GA
guidelines for the recycling and resource utilization of surfaces from the decomposition products of electrolytes
spent GA. Then, the current status of spent GA recycling at low potentials.54 This SEI layer passivates the graphite
was reviewed, including regeneration, secondary applica- surface to allow Li+ transport but to block electrons
tions in other energy storage fields, as raw materials for tunneling, thus preventing the continuous electrolyte
graphene-based materials, and catalysts and functional decomposition and enabling the reversible lithiation/
composite materials. Finally, the current problems and delithiation of the GA. In general, a dense and intact SEI
challenges facing the recycling of spent GA are presented, layer is crucial for the service life and performance of
4 of 27 QIAO ET AL.
F I G U R E 2 The failure mechanisms

of graphite anode in spent lithium-ion
batteries
F I G U R E 3 Failure mechanisms of
solid electrolyte interface (SEI) layers
and the evolution of SEI layers
LIBs.55 However, the SEI layer on the GA surface is increased thickness of the SEI layers. The thicker SEI
chemically unstable and mechanically fragile, and it will layers will increase the ionic resistance. At the same time,
gradually fail during continuous charge–discharge cycles organic compounds (such as lithium ethylene di-
due to mechanical, chemical, or thermal reasons carbonate and lithium ethylene mono-carbonate) in the
(Figure 3).56 SEI layers will also decompose to change the composi-
Upon charging-discharging of LIBs, continuous lithia- tions of the SEI layers, which is the so-called chemical
tion/delithiation of the GA leads to the repeated tensile failure of SEI. On the one hand, the decomposition of
and compressive strains of the SEI layers and thus will organic compounds leads to the increasing concentration
generate cracks in the SEI layers. This phenomenon is of inorganic salts (such as LiF and Li2CO3) in the SEI
usually named the mechanical failure of SEI.57 Electro- layers, making the SEI layers more fragile. On the other
lytes will diffuse through these cracks in the broken SEI hand, the decomposition of organic compounds will pro-
layers to reach the GA surfaces and further decompose. duce gaseous products (e.g., C2H4 and CO2) and soluble
The ongoing electrolyte decomposition will consume organolithium compounds (e.g., lithium methyl carbon-
more Li+ ions to form new SEI layers, leading to an ate and lithium propionate). The escape of gaseous
QIAO ET AL. 5 of 27
F I G U R E 4 Schematic
illustrations of lithium dendrites
(A) The generation of lithium
dendrite. (B) Types of lithium
dendrites morphology.
Reproduced with permission.65
Copyright 2015, IOP Science.
Copyright 1998, Elsevier.
(C) The subsequent
phenomenon of lithium
dendrite after continuous cycles.
Copyright 2017, Springer Nature
products from the SEI layers and the dissolution of orga- 2.1.2 | Lithium dendrites
nolithium compounds into the electrolytes will make the
SEI layers porous. Consequently, the porous SEI layers Lithium dendrites are formed at the anode and grow
are not electrochemically stable enough to protect the toward the cathode during the charging/discharging pro-
GA. Moreover, the decomposition reactions of SEI layers cess of LIBs.58 The constantly growth of lithium dendrites
and electrolytes are exothermic, This is known as the can puncture the separator and make a connection of
thermal failure of SEI. As a result, the thermal failure electrodes, which causing an internal short circuit of
will further aggravate the mechanical and chemical fail- LIBs. The formation of lithium dendrites can be divided
ure of the SEI layers. into three stages (Figure 4A).59 In the first stage, highly
In above, the failure of SEI layer is not unitary but reactive Li+ reacts instantly when it comes into compo-
different failure mechanisms interact with each other nents such as organic solvents in electrolytes, forming
and aggravate the damage of SEI layer jointly. With the SEI film, which is earlier than lithium dendrites. The
failure of SEI, the electrolyte can diffuse through the ideal SEI film is a great ionic conductor, which could pre-
damaged SEI layer to the GA and have side reactions vent further reaction between electrolyte and Li+. How-
with the electrons in GA. The deposition of side reaction ever, in the actual cycling process, Li+ can still pass
products on the surface of GA will not only cause the sur- through the SEI layer and deposits on the anode surface.
face defects of graphite, but also increase the interfacial Furthermore, due to the unstable characteristics of elec-
impedance and hinder the interfacial transport of Li+. trolyte, SEI layers and the influence of charge–discharge
This can reduce the reversibility of charge transfer, make circumstances, the distribution of lithium deposition is
the internal resistance of the battery continue to increase not uniform. Then is the nucleation stage, the continuous
and even lead to battery failure. accumulation of heterogeneous precipitation causes
6 of 27 QIAO ET AL.
bulging in some places until the SEI layer destroyed. The resistance.72 However, this expansion cannot only be
last stage is the growth stage, the growth of lithium depo- explained by the growth of the SEI layer on the surface of
sition continuously exacerbates in the length direction GA. The stress generated during the lithiation and de-
after piercing the SEI film, producing visible dendrites. lithiation process can also facilitate the generation and
Besides, the number of dendrites is mainly dependent on propagation of cracks. In addition, the cracks spread
the nucleation stage, while the morphology of lithium along the grain boundaries of the polycrystalline graphite
dendrites is mainly determined by the growth stage. The (Figure 5). The micro-cracks continuous growth and
morphology of lithium dendrites generally includes four makes the volume of GA further extend.73 The propaga-
types, including whiskers, moss, trees and globules. tion of micro-cracks also leads to the cracking and shed-
(Figure 4B). It is believed that current density has a direct ding of graphite particles. In addition, solvated Li+ and
correlation with the morphology of lithium dendrites and organic solvent embed between the GA layers and the
high current density enhances the growth of lithium den- organic solvent generates gas through the oxidation–
drites.60 The rough globus lithium deposition occurs at reduction reaction between the GA layers. The presence
very low current density (less than 0.1 mA/cm2),61 which of gas further expands the damage to GA particles, which
is a relatively ideal sedimentary morphology because of accelerates the cracking of GA particles or even the exfo-
no sharp cusp. The whiskers dendrites usually formed at liation from the current collector.74
low current density (0.2 mA/cm2),62 the whiskers
diameter broaden and stick to a mossy structure with the
current density increases. High current density 2.1.4 | Copper corrosion
(0.7 mA/cm2) accelerates the growth of lithium den-
drites, which causes the dendrite tips to grow quickly and Copper foil is the most common current collector for
split to generate longer, straighter trees dendrites.62 With anode due to its high conductivity, electrochemical stabil-
repeated cycles, lithium dendrites will be stripped and ity and good mechanical properties.76 It plays an impor-
resulting in dead lithium, thick SEI as well as porous tant role in the electronic exchange between the
electrode finally (Figure 4C).63 Lithium dendrites can sig- electrode materials and the external circuits. Cu current
nificantly expand the interlayer distance of graphite collector faces some challenges during practical applica-
(10%) during the nucleation stage, and the continuous tions, especially the environmentally assisted cracking.77
growth of lithium dendrites can cause dislocation/cracks Therefore, before going to service in commercial LIBs,
of graphite sheets, and even lead to particle breakage.64 Cu current collector needs some pretreatments such as
When the lithium dendrites connect two electrodes, it acid–base etching, corrosion-resistant coating conductive
can cause short circuits and lead to catastrophic failures coating in order to improve the adhesion properties and
and even fires. reduce corrosion rates. These pretreatments have signifi-
cantly help for Cu current collector (Figure 6A). Even so,
copper current collector still suffer corrosion over the
2.1.3 | Particle fracture charging/discharging cycles.78 When the anode electrode
of the LIBs reaches its own high potential, the corrosion
Graphite has a layer structure and the original distance of the Cu current collector by the over-discharging of the
between graphite layers is 0.335 nm.68 In the charging LIBs is inevitable (Figure 6B). After over-discharging to
and discharging process, the interlayer spacing of graph- 0.0 V, about 6% copper is detected on the cathode side by
ite expands to accommodate Li+.69 Previous researches Energy-dispersive X-ray spectroscopy (EDX) analysis
indicated that the interlayer spacing of recovered GA is which demonstrated that dissolved copper (Cu2+) could
about 0.3703 nm,70 which is 10.5% higher than fresh indeed migrate through the separator from the anode
GA. It is revealed that the particle diameter and volume side to the cathode side.79 The dissolve of copper current
expansion increased with the cycling times under at same collector will cause a series of chemical, electrochemical
current density. For example, the average GA particle and electrical phenomena elsewhere in the battery. Cu2+
diameter and volume increases 10% and 30% at can be redeposited on the GA surfaces as Cu metal to
200 cycle times, whereas that is 20% and 70% at form dendrites, which cause surface contamination and
800 cycle times.71 The increase in the size of GA is also damage to the GA.80 The dendrites gradually grow and
due to the formation of SEI in the primary particles or eventually penetrate the separator to connect the anode
the increase in porosity in the secondary particles. The and cathode, causing short circuits and failure of
enlarge of graphite particle volume causes the breakage battery.79,81
and regeneration of SEI film, thus leading to the con- The failure of LIBs is a complex process involving
sumption of electrolyte and the increase of internal multiple factors, including physical, mechanical,
QIAO ET AL. 7 of 27
F I G U R E 5 Schematic
diagram and scanning electron
microscope images of particles
fracture in graphite anode.
Copyright 2011, Elsevier
F I G U R E 6 Schematic diagram and

scanning electron microscope images
(A) Raw copper current collector.
Copyright 2009, Springer Nature.
(B) Copper corrosion. Reproduced with
permission.78 Copyright 2009, Springer
Nature
electrochemical and other aspects evolutions. The fail- without impurity and uniformly distribution. The weak
ure of the battery will have more or less impact on van der Waals forces between two-dimensional layered
GA. Understanding the changes and characteristics of graphitic structures make it easy for ions and molecules
spent GA after failure is an important prerequisite for to be introduced, which is beneficial for the intercalation
its subsequent utilization. Next, the changes occur on and extraction of Li+ and could provide high-rate charge
GA in spent LIBs will be discussed detailed, especially and discharge performance.
in the morphology and structure. Graphite materials have a relatively stable body struc-
ture and a small degree of change during short-term
charging and discharging, but their surface structure will
2.2 | Characteristics of spent GA be attenuated to a certain extent. When the Li+ deinter-
calated at a shallow degree, the surface structure of GA
The typical scanning electron microscope (SEM) images appears the attenuation, and the degree of disorder
of initial GA are shown in Figure 7A, which indicated increases significantly.82 In addition, the locations of
that GA has an obvious layered structure, smooth surface structure attenuation are non-uniformly distributed on
8 of 27 QIAO ET AL.
F I G U R E 7 (A) Scanning electron microscope (SEM) images of natural graphite. Reproduced with permission.94 Copyright 2001,
Elsevier. Reproduced with permission.91 Copyright 2011, Spring Nature. (B) SEM images of GA under 0 and 286 cycles. Reproduced with
permission.85 Copyright 2001, Elseiver. (C) SEM and TEM images of fresh and degraded GA. Reproduced with permission.90 Copyright 2016,
Chen Lin et al. (D) SEM images of GA with cracks. Reproduced with permission.91 Copyright 2011, Spring Nature. (E) SEM images and
Schematic diagram of degraded GA exfoliation. Reproduced with permission.92 Copyright 2021, Spring Nature
the graphite surface. Previous studies have shown that in passivation film with a detectable thickness could be
rechargeable LIBs, GA usually suffers severe surface observed with the naked eye. Furthermore, the harm of
structure damage after long-term cycling.83,84 Li et al.85 overcharge to GA should not be underestimated.86 The
investigated the morphology variation of GA in prismatic morphology and structure of GA during the overcharge
Sanyo UF653467 batteries with a nominal capacity of process were investigated by SEM and TEM.87 It was
930 mAh under charging/discharging cycles. The SEM found that no obvious abnormal feature on the surface of
images (Figure 7B) showed GA consisting of large parti- GA after normal cycling test while the overcharged
cles and some changes occurring on the surface of the cycling graphite shows totally different facial characteris-
anode with cycle times increasing. After 286 cycles, many tics. It is attributed to the lithium dendrites formation
deep cracks appeared on the GA surface, and a and the morphology images indicated that most of the
QIAO ET AL. 9 of 27
structure of the GA is not strongly affected by abuse. peeling may increase the reaction area exponentially,
However, the surface of the GA particles has undergone which will have an adverse effect during the charging/
major changes. This change will cause irreversible capac- discharging cycling (Figure 7E).
ity loss, making it difficult for lithium ions to diffuse into In conclusion, GA from spent LIBs exhibits the fol-
the graphite and accelerating the surface changes. lowing characteristics. First, GA recovered from spent
The structure of GA changes by the repeated Li+ LIBs usually appears severe surface damage. Besides,
intercalation/delamination during the long-term spent GA maintain the layer structure, but the interlayer
charging-discharging cycles. The van der Waals forces spacing is larger than fresh GA and the interlaminar
between graphite layers are weakened and leading stress is weakened. Furthermore, there are some residual
mechanical fatigue. The continuous intercalation/ impurities in GA, including organic binders, metal spe-
delamination of Li+ further aggravates the mechanical cies such as Li, Cu, and trace amounts of amorphous car-
changes and results a larger layer spacing as well as the bon species.93 And the types and contents of residual
volume expansion of GA particles.88 It is believed that impurities in GA of spent LIBs are also different, because
the structural damage is extremely severe during high of the different process formulas and working conditions
current density.62 The local space charge generated by of different manufacturers. Recycling of GA from spent
the excess of positive charges at the GA are easy to cause LIBs is an important approach for turning waste to
an unstable internal structure and induce lithium den- wealth by preventing raw material consumption and
drites.89 The growth of lithium dendrites could be initi- avoiding environmental pollution, which is beneficial for
ated in several different positions of the graphite the sustainable development of the LIBs industry. A
particles, and do not need to correspond to each other.88 detailed discussion of the spent GA recycling is listed in
Internal structure changes and growth of lithium den- the following section.
drites induced a large volume expansion, resulting the
evolution of diffusion induced stresses and mechanical
failure.90 As shown in Figure 7C, the average particle size 3 | RECY CLING O F S PENT GA
was about 100 nm, the edge structure of degraded GA
began to mellow, some circular particles (100–150 nm) Pretreatment processes are essential before downstream
appeared on the surface, and the cracks and fracture can recycling processes of spent LIBs. In order to recycle
be clearly observed in the TEM images. Besides, the spent LIBs more efficiently, many pretreatment methods
highly anisotropic nature of the grains should be noted have been developed. After common pretreatment
particularly, because the insertion of Li+ is anisotropic, methods such as complete discharge,95,96 mechanical
which occurs at the edge of the prism rather than the disassembly,97–100 seperation101,102 and so on, each com-
base planes.91 As shown in Figure 7D, it can be seen that ponent is ready to second recycle treatment. Here, we
the growth of the typical hairline cracks and the bifurca- concentrate on the recycling processes of spent GA.
tion of the cracks in the particles, indicating that the
crack path has anisotropic properties. From surface
defects to trans crystalline cracks, there are pores of 3.1 | Regeneration of GA
different sizes in graphite particles. The presence of
grain boundaries, cracks and pores indicate that if the Some studies have revealed that recovered GA could be
electrolyte can enter into the interior of particles, then regenerated as anode materials for energy storage devices
Li+ can also be carried out by grain boundary/pore dif- after some retreatments.103–106 Low-cost regeneration of
fusion and volume diffusion. In situ synchrotron x-ray GA from spent LIBs is of great significance to solve the
techniques and in situ mass spectroscopy can examine problem of waste graphite utilization and pollution.
the changes occurring on the GA during the heating Comparing with the fresh graphite, the directly recycled
process by tube furnace.92 It is observed that the meso- GA (with coating, SEI layer and other Impurities)
porous graphite with a particle size of 15 μm, PVDF exhibits lower initial discharge capacity, which are 354.2
binder and conductive carbon black are located on the and 298.7 mAh/g respectively. Due to the presence of
graphite surface and gaps. During the heating process, residual impurities, the graphite content in the directly
the lithium flowing out of the graphite lattice will recycled GA is low, leading a low specific capacity.107 In
gather on the edge of the graphite sheet and move in order to restore the initial properties of the spent GA, it is
the in-plane direction. Then, as the temperature rises, crucial to remove the residual impurities in it. Pyrolysis
the gas is released, and the reaction product covers the treatment is a common way to remove impurities before
surface of the anode. At the same time, the violent regenerating the GA from spent LIBs. Cu current collec-
reaction will cause the graphite layer to peel off. The tors melt into spheres by high-temperature smelting, then
10 of 27 QIAO ET AL.
F I G U R E 8 (A) Cycle performance curves of regenerated graphite anode (GA). Reproduced with permission.107 Copyright 2018, Elsevier.
(B) Scheme of GA after different treatment. Reproduced with permission.110 Copyright 2021, Elsevier. (C) The initial charge–discharge
performance and cycling stability for the pilot graphite product and the commercial graphite. Reproduced with permission.111 Copyright
2011, IOP Science
GA and Cu can be completely separated by the sieving needs to be recoated by pyrolytic carbon from phenolic
process. The recovery rate of GA is related to the size of resin. Although regenerated GA with coating layer still
mesh, 77.53% GA can be recovered under 300 mesh. containing residual acetylene black and a little carboxy-
Under 300 mesh, the purity of recovered GA powders is methylcellulose sodium pyrolysis product, it has a little
about 99% while that can reach to 99.5% at 600 mesh, negative effect on the electrochemical performances. The
which meets the standard of anode electrode for LIBs.108 regenerated GA could fully meet the requirements of
Pyrolysis treatment can also remove electrolytes and reuse, and the initial discharge capacity is 377.1 mAh/g
binder, which is beneficial to the following process. All and capacity retention is 98.76% after 50 cycles
the styrene-butadiene rubber, carboxymethylcellulose (Figure 8A), which is higher than the midrange graphite
sodium and most acetylene black can be removed after in the same type.107 By combining advanced microscopy
heat-treated. But at the same time, the coating layer on and spectroscopy techniques, it is noted that although
the GA surface is also damaged, so that heat-treated GA thermal annealing can restore most of the capacity of
QIAO ET AL. 11 of 27
F I G U R E 9 (A) Flow chart of the recycling process, specific surface area, pore size distribution of spent graphite anode (GA) separated
from anode, current collectorrate, rate capacities and cycle performance of regenerated GA. Reproduced with permission.112 Copyright 2019,
Elsevier. (B) Spherical aberration electron microscopy images of spent GA, the cycle performance and rate capacities of prepared samples.
Reproduced with permission.113 Copyright 2020, American Chemical Society. (C) Dissemble of anode materials from spent LIBs, the process
of separation of GA from copper foil, current changes with electrolytic time and the rate capability of recovered GA. Reproduced with
permission.115 Copyright 2021, Elsevier
spent GA, the remaining lithium in GA particles cannot proposed (Figure 8B). Boric acid treatment can not only
completely removed.109 In order to remove the residual repair the composition/structural defects of degraded
lithium completely, boric acid solution pretreatment and GA, but also form functional boron doping on the surface
short-time annealing at medium temperature were of GA particles, ensuring high electrochemical activity
and excellent cycle stability (initial capacity is 330 mAh/g electrochemical activity of graphite. The electrochemical
and retained the capacity after 100 cycles). During the measurements demonstrate that after 100 cycles, the
process, it is also noted that heat temperature will influ- capacity of recycled graphite is 345 mAh/g, which is
ence the crystal lattice restoration of regenerated similar to industrial graphite (347 mAh/g) and also com-
GA. The increase of temperature can accelerate the parable to the products from acid leaching. Moreover,
growth of graphite crystallites and the degree of graphiti- the electrolysis method is also an effective and clean
zation, thereby promoting the close packing and arrange- process to separate copper and GA from spent LIBs
ment of the crystallites. Treating at 3000 C for 6 h is (Figure 9C).115 In this process, Cu foil can be reused
proved to be one of the optimal approaches for eliminat- directly and the residual lithium can dissolve in the elec-
ing the internal stress and achieving the highest degree of trolyte and be recovered by precipitation method. The
graphitization.110 The regenerated GA exhibits great elec- recovered GA shows excellent cycling stability and rate
trochemical properties and the capacity retention rate is capability (427.81 and 350.47 mAh/g). Meanwhile, it also
97.3% after 1000 cycles while the initial capacity is shows excellent rate performance and the specific capac-
352.5 mAh/g (Figure 8C). Furthermore, after 1600 cycles, ity recovered to 347 mAh/g after a high rate.
the release capacity of the product is 351.9 mAh/g, and
the capacity retention rate is 87.88%.
Pyrolysis treatment not only needs high temperature 3.2 | Reuse in other energy storage
but also generates toxic gases, which leading to high devices
energy consumption and air pollution. Therefore, some
chemical solvents have also been employed to avoid high In addition to being repaired and regenerated and re-
energy consumption and obtain pure GA in the recovery. used in LIBs, the recycled GA can also be used in other
Yang et al. proposed an acid leaching method to regener- energy storage systems after treatment, such as lithium-
ate pure GA after a two-stage calcination.112 After being sulfur batteries, sodium-ion batteries, potassium-ion bat-
leached in 1.5 M HCl solution, almost 100% lithium, teries68 and super capacitors.116 The GA from spent LIBs
98.5% copper and 99.2% aluminum were dispersed in the has two special characterizations to enhance trapping
leaching solution. In addition, lithium was recovered as and catalytic performance toward polysulfides. On the
lithium carbonate with a purity of up to 99% by adding one hand, the porous structure and defects formed in the
sodium carbonate to the leaching solution. It is found repeated lithiation-intercalation process can provide
that regenerate GA has high initial specific capacity at many adsorbent sites to limit the soluble polysul-
37.2 mAh/g (591 mAh/g), 74.4 mAh/g (510 mAh/g) and fide.117,118 At the same time, due to the decomposition of
186 mAh/g (335 mAh/g). The retention rate after the electrolyte, several polar functional groups are pro-
100 cycles is as high as 97.9%, and it also shows excellent duced on the graphite surface, which is beneficial to the
cycle performance at a high rate of 372 mA/g adsorption of polysulfide and the wetting of the electro-
(Figure 9A). To further improve the purity of regenerated lyte.119 On the other hand, due to the dissolution of the
GA, a systematic approach combined sulfuric acid curing, active cathode material, transition metal elements such
leaching and calcination were proposed.113 Comparing as Ni, Co, and Mn are introduced into the waste GA,
with direct acid leaching, sulfuric acid solidified acid which can also fix polysulfides, improve conductivity,
leaching has a higher impurity removal efficiency, which and promote polysulfide conversion kinetics.120 A spent-
the purity of recovered GA can reach to 99.6%. Besides, graphite-based interlayer is developed to reduce the
the regenerated graphite is close to unused commercial “shuttle effect” in high-performance lithium-sulfur batte-
graphite in both morphology and structure. It also shows ries (Figure 10A).121 The discharge capacity of lithium-
an excellent electrochemical performance in terms of sulfur batteries using spent GA modified separators can
charging capacity and cycling. The retention rate can reach to 968 mAh/g, the attenuation rate at 1C is 0.08%,
reach 98.8% when the initial charge capacity is 349 mAh/g, and the discharge times can reach more than 500 times.
which proves the feasibility of recycled GA used in LIBs In addition, the spent GA and sulfur composite can be
(Figure 9B).113 Inorganic acids are demanding to handle, considered as the cathode material for lithium-sulfur bat-
harmful to the environment, and prone to produce second- teries.120 And compared with commercial graphite, the
ary pollution. In order to meet the needs of environmentally cathode has an excellent cycling performance, with an
friendly development, green chemical solvents have been average capacity decay of only 0.006%/cycle after
used to replace inorganic acid. Wang et al.114 found that 500 cycles. Spent GA also shows great potential as anode
water can react with the residual lithium in GA to precipi- material in lithium-ion capacitors (LICs) due to its larger
tate hydrogen, which can separate the thick SEI from GA d-spacing than commercial graphite.122 Before the fabri-
and remove most of the impurities and restore the cation of LICs, GA was pre-lithiated (LiC6) into a
F I G U R E 1 0 (A) The schematic illustration of the adsorption properties and catalytic effects of a graphite anode (GA)-modified
separator in lithium-sulfur batteries; the electrochemical performances of lithium-sulfur batteries with different separators. Reproduced with
permission.121 Copyright 2021, Royal Society of Chemistry. (B) The morphology features of GA, cyclic performance of the dual carbon LICs
at different temperatures, and Nyquist plots for the electrochemical impedance spectroscopy analysis for the assembled dual carbon lithium-
ion capacitors before and after cycling, in which the circles relate to the experimental data and the lines corresponds to the fitting values.
Reproduced with permission.122 Copyright 2013, Royal Society of Chemistry. (C) Schematic diagram of the synthesis process for recycled
nagative graphite and scanning electron microscope images. Reproduced with permission.125 Copyright 2022, Elsevier
graphite intercalation compound for supplying Li+. The density and maximum power are 59.93 and 6.8 kW/kg,
dual carbon LICs based on GA/LiC6 anode material respectively. Furthermore, it has a capacity retention rate
shows an energy density of 185.5 Wh/kg at a power of of approximately 98% after 5000 cycles. Some studies
0.319 kW/kg under room temperature (Figure 10B). have revealed that recovered GA can also be considered
Unlike lithium embedding, sodium embedding in as an anode for sodium ion batterires.124 The results indi-
graphite is extremely limited due to the large size. Spent cated that recovered GA displayed excellent rate perfor-
GA is considered as a pre-sodiated anode for Na-ion mance in both half-cell and full-cell. Meanwhile, it also
capacitor, therefore it can provide higher energy density has a stable capacity retention of 84% and 78% after
than commercial graphite.123 The maximum energy 100 cycles, respectively.
F I G U R E 1 1 (A) Scanning electron microscope (SEM), transmission electron microscope images of GA from spent lithium-ion batteries
(LIBs) and graphene prepared by graphite anode (GA). Reproduced with permission.133 Copyright 2018, Elsevier. (B) FTIR spectra of
prepared samples. Reproduced with permission.134 Copyright 2019, Springer Nature. (C) High resolution transmission electron microscopy
(HRTEM) and atomic force microscopy (AFM) of glucose thermal treated graphene. Reproduced with permission.135 Copyright 2021,
Chemistry Europe. (D) The schematic diagram for different treatment of GA. Reproduced with permission.136 Copyright 2018, American
Chemical Society. (E) Flow diagram for the synthesis of reduced graphene oxide (RGO) with recovered materials from spent LIBs.
Reproduced with permission.116 Copyright 2018, Elsevier. (F) Schematic diagram for the formation of soluble graphene. SEM images of
graphene under different temperature and TEM images of graphene under 400 C. Reproduced with permission.138 Copyright 2018, Springer
Nature
In addition, spent GA also has great potential in dual- and inert gas atmosphere heating treatment was pro-
ion batteries. As shown in Figure 10C, a two-step method posed.125 The expanded layer spacing of spent GA was
of regenerating spent GA by anhydrous ethanol cleaning restored through reconstructing the crystal structure and
morphology by heating process. The recycled negative has been restored (Figure 11B). And the characterizations
graphite not only has reduced disordering but also also demonstrate that the prepared RGO exhibits obvious
exhibits a good layered structure, which facilitates Li+ layered structures, smooth and ordered surface texture,
transport. Electrochemical results demonstrated that the wide interlayer spacing as well as small resistivity. Glu-
recycled negative graphite applied to dual-ion batteries cose was also considered as a reductant to prepare high-
exhibited a comparable specific capacity to that of com- quality graphene sheets.135 As shown in Figure 11C, the
mercial graphite (about 87 mAh/g). In addition to recy- size of prepared RGO is about 5 μm and the thickness
cling GA alone, Du et al.126 proposed a novel method to ranges from 0.82 to 1.09 nm. Moreover, the yield of RGO
recover both lithium ferro phosphate (LFP) cathode and is about 84.3% and the number of layers ranging from
GA from used batteries, considering the excellent stabil- 2 to 9 which was calculated by measuring thickness of
ity of LFP and the high electrical conductivity of graphite. 45 flakes.135 Except for adding extra reducing agents, the
The recovered cathode and anode mixture was used as Al current collector and stainless steel shell from spent
the cathode in a new type of dual-ion battery to store LIBs can also be reducing agents to prepare RGO
both anions and cations. The hybrid cathode combines (Figure 11D).136
the advantages of both LFP and GA, and exhibits a good When preparing RGO by the Hummers method, the
electrochemical performance, which the reversible capac- consumption of acid solution and oxidizing agent is an
ity is about 130 mAh/g at 25 mA/g. important factor from both environmental and economic
considerations. Due to the existence of structural defects
in GA, the consumption of H2SO4 and KMnO4 are about
3.3 | Graphite based materials 40% and 28.6% less than that of natural graphite respec-
tively.137 Besides, GA from spent LIBs has the character-
Graphene is a single-atom-thick carbon sheet with sp2 istic of irregular expansion after the Li+ intercalation and
structure,127 which has attracted massive attention due to deintercalation during the charge–discharge cycles, and
its fascinating electronic, thermal and chemical proper- this prefabrication process facilitated the exfoliations of
ties and has potential in the nanocomposite, sensors, graphite both in chemical and physical. Shear mixing can
microelectronics, thin films, micro-electrical devices and enhance the expansion which increase the productivity
other applications.128–130 Recently, GA from spent LIBs of graphene by four times.136 Furthermore, acid treat-
have been employed to prepare graphene and graphene ment can further expand the GA lattice and increase the
oxide (GO) because of their special structure especially yield of RGO to 83.7%, which is 10 times higher than that
large layer spacing.131,132 The Hummers method is one of of normal graphite (Figure 11E).In addition to traditional
the most common methods to prepare GO and reduced GO, soluble RGO nanosheets can also be prepared by
graphene oxide (RGO). The acid solution was used to spent GA from LIBs.138 NaOH and KOH eutectic solvent
remove the metal impurities on spent GA, and a mesh was used to reduce the GO prepared by spent GA
sieve was employed to uniform the particles size.133 through the Hummers method. And the unsaturated
Through the Hummers method, GO and RGO were pre- oxygen-containing part on GO sheets can be effectively
pared by spent GA and commercial graphite, respec- removed. As shown in Figure 11F, RGO prepared under
tively. After thermal explosion and exfoliation of solidly different temperatures are in different degree of disor-
stacked graphene layers, the specific surface area of RGO dered and wrinkled. Furthermore, the higher the treated
increased from 36.2 to 362.4 m2/g (Figure 11A). Further- temperature is, the worse the disorder of RGO is. The
more, the specific surface area of RGO prepared by GA is prepared soluble RGO dispersed in water or ethanol
8% higher than that prepared by commercial graphite. exhibit excellent stability, and no visible settlement after
This result indicates that spent GA from LIBs could pro- gravity standing for 4 weeks. The excellent dispersibility
vide a larger surface area than commercial graphite of soluble RGO has wide potential applications in many
under the same condition. To reduce environmental pol- areas such as energy, chemical industry and micro-
lution, Yang et al.134 proposed an ultrasonic assistant electronics.
method to separate GA from copper foil with water as a In addition to Hummers method, other methods have
solvent. Then the collected GA was prepared into GO also been employed to prepare GO or RGO by spent GA
through a modified Hummers method. And vitamin C from LIBs. A one-pot redox reaction method is suggested
was used to replace the traditional agent to reduce the to prepare RGO using a ternary system containing
GO into graphene. The fourier-transform infrared spec- H2SO4, KMnO4, and C2H4O3.139 This method can not
troscopy (FTIR) measurements indicates that vitamin C only avoid the subsequent reducing agents and other
has good reducibility, a number of oxygen-containing high-temperature reduction processes but also has a high
groups have been removed, and the structure of graphene yield of 61.2%. The electrochemical method has also been
F I G U R E 1 2 (A) Schematic diagram of the recycling process for waste mixed cathode material with graphite anode (GA) as reductant.
Reproduced with permission.143 Copyright 2020, Elsevier. (B) A typical microstructure of a quenched sample. Reproduced with
permission.144 Copyright 2020, MDPI. (C) Preparation diagram for magnesium hydroxide-modified mesocarbon microbeads composite.
Reproduced with permission.149 Copyright 2016, American Chemical Society. (D) Schematic diagram and scanning electron microscope
images of MnO2 modified GA materials. Reproduced with permission.150 Copyright 2019, American Chemical Society. (E) The degradation
rate of on methylene blue by CuO and GA-Cu composite. Reproduced with permission.152 Copyright 2018, Springer Nature
widely used in preparing graphene in recent researches. because NaCl can enhance the hydrolysis process of
Graphene produced by electrochemical exfoliation water due to its high electrical conductivity, resulting in
method is easy to agglomerate, so that surfactants are an enhancement of the edge exfoliation of graphite to
added to avoid this phenomenon. The type of aqueous produce graphene. The Z-height profiles obtained from
electrolytes containing different surfactants (cationic, AFM images demonstrates that the exfoliated samples
nonionic and anionic) can make influences on electro- contained only a few-layer graphene sheets. Kang
chemical exfoliation process.140 It is also found that the et al.141 creatively proposed a short-circuit discharge
addition of NaCl in electrolytes could increase the yield method to prepare large-size GR sheets. This method
of graphene compared with that in pure surfactants elec- including two steps, the lithium intercalated graphene
trolyte systems during the graphite exfoliation. This is compound was first obtained after the short-circuit of
LIBs, then the compound was exfoliated into graphene reaction is higher than that of commercially available
by ultrasonic. The prepared graphene has the characteris- nitrogen graphene because of the presence of carbon
tics of large size, few defects, single layer or less than vacancies and higher content of active nitrogen on the
three layers. Compared with electrochemical methods surface of graphene. From these results, it is clear that
reported in the literature, the quality of graphene has GA from spent LIBs could be recycled and reutilized in
been significantly improved and the yield can reach to the catalyst.
8.76%. Furthermore, the battery-grade Li salt also can be In addition, GA also exhibits an effective catalytic
efficiently recovered as by-product.142 The lithium graph- ability on the adsorption enhancement of water pollu-
ite intercalation compounds were obtained from re- tion. For example, the GA compound modified with
charge the spent LIBs, then they were into a hydrolysis nanoscale Mg(OH)2 on surface was employed to remove
procedure which the expansion/micro-explosion mecha- excessive phosphate, which can lead to freshwater eutro-
nism could make it to graphene. Meanwhile, lithium was phication and deterioration of aquatic ecosystems
simultaneously recovered in the form of battery-grade (Figure 12C).149 The adsorb quantity can reach to
lithium carbonate in the above process. According to eco- 588.4 mg/g, which is one order higher magnitude higher
nomic analysis, the production cost of graphene prepared than previously reported carbon-based adsorbents. Fur-
by GA was extremely low ($540/ton) compared to that of thermore, GA also exhibits adsorption ability on heavy
commercial graphene. It is indicated that preparing gra- metal polluted water containing plumbum, cadmium,
phene by spent GA in LIBs cannot only alleviate the and silver. To improve the sorption ability, MnO2 nano-
shortage of natural graphite but also has huge economic particles can be loaded to the supporting GA by a facile
benefits. hydrothermal method. Compared with single GA pow-
der, the MnO2-modified GA exhibits a higher removal
rate on plumbum, cadmium and silver, which reach to
3.4 | Catalyst 99.9%, 79.7% and 99.8%, respectively (Figure 12D).150 In
order to further evaluate the adsorb ability of GA,
GA also has attracted some attention on catalyst and Nguyen et al.151 conducted batch adsorption experi-
reduction areas due to its economic and abundant yield. ments on cadmium, barium, 2,4-dinitrotoluene (DNT),
Pindar et al.143 proposed a short duration, cost-effective 2,4,6-trinitrotoluene (TNT), hexahydro-1,3,5-trinitro-
recycling process for waste mixed cathode material 1,3,5-triazine (RDX), and 2,4-dichlorophenol (DCP). In
(Figure 12A). It is worth mentioning that GA was crea- addition, the catalytic performance of GA in thiol (-SH)
tively used to improve the metal extraction rate in reducing agent, dithiothreitol (DTT) and hydrogen sul-
cathode materials as a reductant during the microwave- fide (H2S) reduction of DNT and RDX and persulfate
assisted method. Moreover, GA shows better-reduced oxidation were also investigated. The results demon-
ability on lithium cobalt oxides and lithium nickel man- strate that GA has better adsorption performance for
ganese oxide than activated charcoal, which avoid addi- toxic metals compared with other types of carbonaceous
tional external reductants in the recycling process. Based materials. And in the oxidation and reduction process, it
on this phenomenon, experiments on GA to replace con- has shown a strong ability to promote redox reactions,
ventional reducing agent coke during the nickel slag which indicates that it may be suitable for environmen-
cleaning process were carried on.144 Rapidly reduction tal remediation. To comprehensive reutilize spent LIBs,
results were obtained in the conditions of combination GO-Cu composite material was prepared due to the defect
with GA. Just in the 5 min reduction process, the structure of GA and copper foil from spent LIBs. The com-
valuable metals Co, Ni and Cu were distributed in the posite exhibits a better catalytic photodegradation perfor-
iron-rich alloy, and the remaining Mn and Al in the foam mance on methylene blue than CuO (Figure 12E).152 These
part were discharged into the slag (Figure 12B). Previous studies provide the possibility to recycle GA for synthesizing
studies have shown that graphene-based materials have high-efficiency adsorbents from spent LIBs, which is an eco-
excellent oxygen reduction reaction performance in alka- nomical and environmentally friendly method for heavy
line media, especially when they are doped with hetero- metal polluted water treatment and waste recycling.
atoms such as nitrogen, sulfur, boron or fluorine.145–147
Therefore, high nitrogen doped graphene with uniform
distribution of carbon, nitrogen and oxygen was prepared 3.5 | Functional composite materials
by GA from spent LIBs.148 X-ray diffraction (XRD),
Raman and X-ray photoelectron spectroscopy (XPS) mea- Based on the special structure and performance of GA
surements indicate that the electrocatalytic activity of from spent LIBs, researchers explored and investigated
synthetic nitrogen-doped graphene for oxygen reduction some potential applications of spent GA experimentally,
F I G U R E 1 3 (A) The mechanical properties of the graphite anode (GA) with polypropylene and polyethylene nanocomposite thin films.
Reproduced with permission.153 Copyright 2015, Elsiver. (B) H2 adsorption and CO2 adsorption of RGO prepared by GA. Reproduced with
permission.154 Copyright 2013, Royal Society of Chemistry
especially as functional composite materials. It is noted compared with pure polypropylene and polyethylene, the
that GA could indeed improve the mechanical properties specific conductance of prepared nanocomposite films is
of the polymer film. The composite films are synthesized increased by 5–6 orders of magnitude, which is a good
by recycled GA through a solution intercalation substitute for the commercial graphite and polymers for
method.153 The tensile strength of graphite composite the synthesis of the polymer-nanocomposite thin film.
film combined with polyethylene and polypropylene is Furthermore, GA has also been used as the carbon source
10 times higher than original polyethylene and polypro- for the application in gas storage capabilities like N2, H2,
pylene film, which was increased from 3.0 to 38.1 and 3.4 and CO2. For that, hollow carbon spheres were synthe-
to 33.9 MPa respectively (Figure 13A). Meanwhile, sized by a one-step carbonization process, and RGO was
prepared by GA with Al cases as a reductant From the above discussion, the continued growth of LIBs
(Figure 13B).154 The generated RGO exhibits good gas used in consumer electronics, electric vehicles and grid
storage performance for both H2 and CO2. It also shows a power storage will increase the demands for graphite
superior CO2 uptake capacity of 61.17 cm3/g, while the material. The increase in demand for electric vehicles
H2 storage capacity can reach 200.46 cm3/g at 77 K, will be partially but not fully offset by changes in LIBs
which is greater and comparable to the other literature such as new anode using silicon162 or titanite.163 There-
reports.155,156 Moreover, GA can be used as nanoparticles fore, recycling of GA from spent LIBs has been applied as
in the heat transfer medium. We presented a facile an effective approach to achieve the predicted demand of
freeze–thaw ultrasonic assisted circulation method to battery-grade graphite. Although there has been some
prepare two-dimensional low-layer graphite flakes using progress on the recovery, regeneration and reuse of GA,
GA from spent LIBs.157 GA was easier to exfoliate to pre- there is still a need for developing new and effective
pare low-layer graphite flakes than commercial graphite methods to meet changing recycling needs. Besides,
and the prepared also exhibited a better thermophysical future development in spent GA recycling till faces some
performance in nanofluids than base fluids. challenges based on the existing experience and predic-
Overall these studies, GA from spent LIBs has been a tion. More efforts should be made from the following
potential candidate of carbon source in various applica- aspects to improve the development of GA recycling:
tions. Furthermore, the potential on other application
areas should be explored considering the special structure 1. The purity of recovered graphite should have a certain
and performance of GA. And the recovery of GA should evaluation standard. In the recycling process, metal
obtain more attention from researchers for that the reuti- impurities including residual lithium, binder, and bro-
lization of GA is a win-win opportunity for both resource ken copper foil or the fragments of the cathode mate-
shortage and environmental pollution. rial are possible appear in the recovered GA. The
Among the methods mentioned above, they are cur- impurities can affect the purity of GA seriously and
rently focused on laboratory scale and are still have some hander its next applications. Therefore, the purity of
distance away from commercial production. The pyro- recovered GA should be ensured before reuse in fur-
lytic regeneration of spent GA has great potential in com- ther applications.
mercial production, especially with s the normal end of 2. It also should be noted that the recovered GA surface
life LIBs. Because of its stable change and easy handling, damage is influenced by the aging mechanism like
it can continue to be applied to energy storage systems SEI formation and intercalation of solvent molecules
without excessive processing. Besides, the graphene mar- which lead to surface changes and graphite degrada-
ket is also gradually expanding and relatively mature for tion. Thus, effective surface treatments are needed to
industrialization due to the wide range of graphene appli- remodify the surface structure, reduce irreversible
cations.158,159 Spent GA has been proved to have the capacity loss and improve the capacities.
advantages of low cost consumption and high yield in the 3. The recovered GA is not only limited to the applica-
process of graphene preparation. Therefore, it has a broad tions of LIBs and capacitors, but can also be extended
market prospect as a graphene raw material and can be to sodium batteries and capacitors, and it is also possi-
applied on a large scale. In addition, the application ble to explore as electrode materials for emerging
method of spent GA in other fields is relatively compli- energy storage systems, such as potassium ion batte-
cated, and a mature industrial chain foundation has not ries, super capacitors, aluminum ion batteries, and
yet been formed so that it will take some time to develop flow batteries, and so forth. In addition, graphite and
and grows. its derivatives not only have great application value in
clean energy but also can extend to other aspects such
as gas storage, catalytic reduction reaction as well as
4 | C HA L LEN G E S AN D membrane area. So that the recycling and retreating
P R O S P EC T S techniques of GA need to be multivariate, in-depth
and targeted.
Previous studies demonstrates that the extraction rate of 4. Besides, the price of graphite recovery should be cal-
valuable metals and other useful materials could reach culated in an appropriate way to maximize the econ-
almost 100% in spent LIBs. However, the recycling and omy. Therefore, environmentally friendly, less time
reutilization of waste GA in spent LIBs is of equivalent and cost consuming approaches are more receptive.
importance to that of cathode materials. Because of the
great large demand for graphite in batteries, the Based on the above points, we tentatively propose a
United States and the European Union countries have guideline for the recycling process of spent GA based on
proposed graphite as a key material for recycling.34,160,161 the previous researches and our own insights. First of all,
reduce the dependence on overseas graphite source and

ensure the sustainable supply chain of graphite. Recy-
cling and resourceful utilization of GA should attract
continuous attention for economic and environmental
considerations. The recycling process needs to emphasize
the principles of 3R (Reduction, recovery and reutiliza-
tion)164 and 3E (energy, environment and economy)165
have been suggested. Here, we proposed a new principle
called 3 S, which presents systematic, security and sus-
tainability. For that, the recovery process of GA from
spent LIBs should be systematic, disassemble, remake
and reuse stages are coherent step by step. Especially in
commercial production, manufacturers should classify
spent LIBs into normal spent LIBs and severely damaged
LIBs after safety failures. Then it is sent to different recy-
cling systems, which can realize the step-by-step utiliza-
tion of spent GA in different degrees. A low-cost, simple
and effective recovery system should be designed for the
waste graphite with a lesser degree of failure to help
improve economic benefits. Security emphasizes the
F I G U R E 1 4 Challenges and suggesting principles of spent
safety during the whole recycling process of spent GA,
graphite anode (GA) recovery
there are more safety hazards in the recycling of used bat-
teries, such as incomplete discharge, short circuit and
according to the failure of spent LIBs, they should be battery breakage, especially the high risk in the process
roughly divided into two types, normal spent LIBs with of disassembly which are potential to cause a fire and
limited service life and severely damaged LIBs due to explosion. Therefore, the environment and atmosphere
obvious safety failures. The structure changes on GA in of the workshop should be strictly required to avoid the
natural scrap LIBs are relatively stable, and the main risk of combustion and explosion caused by a large
change is the expansion of interlayer spacing. Simple and amount of GA stacked or electrolyte volatilized in large
effective methods (solvent leaching and heating treat- quantities together. In addition, in view of the pneumo-
ment) can restore its lattice and lamellar structure, coniosis hazards caused by graphite, the health and safety
enabling its secondary application in energy storage sys- of the staff in the recycling site should also be taken into
tems. In severely damaged LIBs, the surface or structure consideration. Sustainability means that the process
damage and impurity doping are complex due to the vari- should be a beneficial development from the resource,
ous failure mechanism, and it is impossible to perform environmental and economic perspective. Considering
simple and unified repairs. In short, recycling of spent the increasing energy crisis and environmental pollution
GA should be targeted and utilized step by step. Spent problems, the recycling process of spent GA should pay
GA without seriously affected should be given priority to attention to the recycling of the instrumentation or
regeneration, and those are severely damaged are more reagents used to avoid secondary pollution and waste of
suitable for secondary processing as raw materials, and resources. In addition, all components of spent LIBs
can be used in related fields by taking advantage of their should be considered for recycling, instead of focusing
advantages. only on the much-noticed electrode materials, in order to
promote the overall sustainability of spent LIBs. In the
future, the recycling of GA is promising to achieve the
5 | S UM MA R Y closed-loop development of in spent LIBs industries
(Figure 14).
In above, spent GA increasing with the continued growth
of LIBs. Despite graphite resource is not as short as other AUTHOR CONTRIBUTIONS
metal resources, it should be noted that not all kinds of Yu Qiao: conceived and designed the project, writing –
graphite can be employed as anode. The recovery original draft, writing-review & editing. Huaping Zhao:
approaches of GA with high performance and high yield conceived and designed the project, writing – original
purity are necessary for resource shortage and environ- draft. Yonglong Shen: Conceptualization, writing-
mental pollution. Moreover, the recycling of GA can review & editing, supervision. Liqiang Li:
Conceptualization, writing-review & editing, supervision. 13. Wei Y, Yang B, Wang S, et al. Vacancy–vacancy pairs induced
Zhonghao Rao: Conceptualization, writing-review & new phase formation in carbon boride: a design principle to
editing, supervision. Guosheng Shao: Conceptualiza- achieve superior performance Li/Na-ion battery anodes.
EcoMat. 2022;4(1):12150.
tion, writing-review & editing, supervision. Yong Lei:
14. Heid, B, Kane S, Schaufuss P. Powering up sustainable energy:
Conceptualization, writing-review & editing, supervision, Building a more Sustainable Battery Industry. McKinsey Quar-
project administration and funding acquisition. terly; 2020.
15. Tran MK, Rodrigues MF, Kato K, Babu G, Ajayan PM. Deep
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Qiao appreciates the support from the China Scholarship
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method to prepare Pd-doped carbon aerogels for hydrogen stor- Zhonghao Rao is a professor and
age. RSC Adv. 2015;5(27):2966-2971. doi:10.1039/C4RA16505E Dean of School of Energy and Envi-
156. Sterlin Leo Hudson M, Raghubanshi H, Awasthi S, et al. ronmental Engineering at Hebei Uni-
Hydrogen uptake of reduced graphene oxide and graphene versity of Technology. Rao was
sheets decorated with Fe nanoclusters. Int J Hydrog Energy. shortlisted for 2020 Clarivate highly
2014;39(16):8311-8320. doi:10.1016/j.ijhydene.2014.03.118 cited Researchers, 2021 Elsevier
157. Yu Qiao WSCH. A facile freeze–thaw ultrasonic assisted circu-
Highly Cited Chinese Researchers,
lation method of graphite flakes prepared by anode graphite
from spent lithium-ion batteries for application in nanofluids.
and World's Top 2% Scientists 2022. He serves in Edi-
Sustainable Energy Fuels. 2021;5(19):4882-4894. doi:10.1039/ tor Boards of Journal of Mining Science and Technol-
D1SE00973G ogy, Energy and Built Environment, Thermal Science,
158. Maio A, Pibiri I, Morreale M, Mantia F, Scaffaro R. An over- Scientific Reports, and Plos One and was guest editors
view of functionalized graphene nanomaterials for advanced of International Journal of Photoenergy, Journal of
applications. Nanomaterials. 2021;11(7):1717. doi:10.3390/ Thermal Science, Frontiers in Energy Research, and
nano11071717
Energies. Prof. Rao also served as the session chair or
159. Wu S, Qureshi T, Wang G. Application of graphene in fiber-
Co-Chairmen of the international conferences several
reinforced cementitious composites: a review. Energies. 2021;
14(15):4614. doi:10.3390/en14154614 times. He is devoted to research on topics including
160. Feytis A. The bright side of graphite. Ind Miner. 2010;7:31-39. energy storage, battery thermal management, thermal
161. Olivetti EA, Ceder G, Gaustad GG, Fu X. Lithium-ion battery safety, multiphase flow and heat transfer enhance-
supply chain considerations: analysis of potential bottlenecks ment. He has over 150 publications in peer reviewed
in critical metals. Joule. 2017;1(2):229-243. doi:10.1016/j.joule. international journals to his credit. The total citations
2017.08.019 is more than 6700/9700 (source: Web of Science/
162. Zuo X, Zhu J, Müller-Buschbaum P, Cheng Y. Silicon based
Google Scholar), and h-index is 41/51.
lithium-ion battery anodes: a chronicle perspective review.
Nano Energy. 2017;31:113-143. doi:10.1016/j.nanoen.2016. Guosheng Shao is Professor and the
11.013 Director of the State Centre for Inter-
163. Zhang L, Zhang X, Tian G, et al. Lithium lanthanum titanate national Cooperation on Designer
perovskite as an anode for lithium ion batteries. Nat Com-
Low-carbon and Environmental
mun. 2020;11(1):3490. doi:10.1038/s41467-020-17233-1
164. Harper G, Sommerville R, Kendrick E, et al. Recycling
Materials (CDLCEM). He is also
lithium-ion batteries from electric vehicles. Nature. 2019; Founding Director of the Zhengzhou
575(7781):75-86. doi:10.1038/s41586-019-1682-5 Materials Genome Institute (ZMGI,
165. Wang Y, Yu Y, Huang K, Tang B. From the perspective of bat- 2016), and Visiting Professor to the University of Sur-
tery production: energy–environment–economy (3E) analysis rey, UK (2018). He earned his PhD in materials sci-
of lithium-ion batteries in China. Sustain For. 2019;11(24): ence at the University of Surrey in 1995 and
6941. doi:10.3390/su11246941
thereupon worked as a research fellow and senior
research fellow, until transferring to the Brunel Uni-
AUTHOR BIOGRAPHIES versity as Reader in Materials in 2005. He joined the
University of Bolton as Professor of Materials Model-
Yu Qiao is on a successive postgrad- ing and Simulation in 2007, and then established the
uate and doctoral program of study Institute for Renewable Energy and Environmental
in the China University of Mining Technologies (IREET, 2011) as its founding Director,
and Technology. She is currently together with the responsibility as Head of Engineer-
being sponsored by China Scholar- ing etc. His academic interest is “designer” materials
ship Council (CSC) as a visiting PhD and application devices, using a materials genome
candidate at Technology University approach to facilitate cost-effective development of
of Ilmenau under the supervision of Prof. Yong Lei. novel materials. His current focus is mainly on sus-
Her research interests focus on the recycling of spent tainable (renewable) energy systems and environmen-
lithium-ion batteries. tal technologies.
Yong Lei is a Professor and Head of nanostructures. He received a few prestigious funding
Group (Chair) of Applied Nano- in Europe and Germany such as two European
Physics at the Technical University Research Council Grants. Lei is an Advisory Board
of Ilmenau, Germany. He started to Member or Associate Editor of a few journals such as
work in Germany as an Alexander Advanced Energy Materials, Energy & Environmental
von Humboldt Fellow at Karlsruhe Materials, InfoMat and Carbon Energy.
Institute of Technology in 2003.
From 2006, he worked at University of Muenster as a
group leader and Junior Professor. In 2011, he joined
the Technical University of Ilmenau as a Chair Profes- How to cite this article: Qiao Y, Zhao H, Shen Y,
sor. His research focuses include template nanostruc- et al. Recycling of graphite anode from spent
turing, energy conversion and storage devices, and lithium-ion batteries: Advances and perspectives.
optoelectronic applications of functional EcoMat. 2023;5(4):e12321. doi:10.1002/eom2.12321
© 2023. This work is published under
http://creativecommons.org/licenses/by/4.0/(the “License”). Notwithstanding
the ProQuest Terms and Conditions, you may use this content in accordance
with the terms of the License.

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Received: 8 November 2022 Revised: 18 December 2022 Accepted: 28 December 2022

Recycling of graphite anode from spent lithium-ion

Yu Qiao 1,2 | Huaping Zhao 2 | Yonglong Shen 3 | Liqiang Li 4 |

EcoMat. 2023;5:e12321. wileyonlinelibrary.com/journal/ecomat 1 of 27

1 | INTRODUCTION points of view, there is of great significance to recycle

F I G U R E 2 The failure mechanisms

F I G U R E 6 Schematic diagram and

reduce the dependence on overseas graphite source and

155. Zhong M, Fu Z, Yuan L, et al. A solution-phase synthesis

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