Resources, Conservation & Recycling 201 (2024) 107326

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Resources, Conservation & Recycling

journal homepage: www.elsevier.com/locate/resconrec

Recycling of spent lithium–ion battery graphite anodes via a targeted

repair scheme
Kechun Chen a, Yuan Ding a, Liming Yang a, *, Zhihao Wang a, Haoxuan Yu a, Difan Fang a,
Yufa Feng a, Liying Hu b, Chenxi Xu c, Penghui Shao a, Xubiao Luo a, d, Liang Chen b, *
a
National–Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063,
China
b
Key Laboratory of Hunan Province for Advanced Carbon–based Functional Materials, School of Chemistry and Chemical Engineering, Hunan Institute of Science and
Technology, Yueyang, 414006, China
c
College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan, 410082, China
d
School of Life Science, Jinggangshan University, Ji’an, 343009, China

A R T I C L E I N F O A B S T R A C T

Keywords: When lithium–ion batteries (LIBs) reach the end of their life, a lot of hazardous wastes will be generated. Un­
Lithium–ion batteries fortunately, the recovery of spent graphite (SG) anodes is always neglected despite the rather high production
Spent graphite cost of battery–grade graphite. In this work, we for the first time propose a novel targeted repair scheme by
Failure characteristic
systematically characterizing and analyzing the structure and composition of SG. The results show that the repair
Targeted repair
Electrochemical performance
scheme achieves effective SG repair and the repaired graphite anode displays excellent lithium storage perfor­
mance, which can be comparable to that of commercial graphite. In addition, the scheme is evaluated to reduce
energy consumption by 79 % and harmful pollutant emission by 90 % as compared to previously reported so­
lutions. Obviously, our work provides a feasible solution for the recovery of graphite anodes from spent LIBs by
understanding the failure characteristics of graphite anodes.

1. Introduction been proposing in the field of academia and industry (Shi et al., 2019;
Chi et al., 2021; Xu et al., 2020). It can be found that many works on the
With the growing of pressure from energy depletion and environ­ recovery and recycle of LIBs focus on the cathodes (such as LiFePO4 and
ment pollution, more and more new energy vehicles have been put into LiCoO2) (Fan et al., 2022; Tran et al., 2019; Chen et al., 2021), but
the market. It is estimated that by 2035, vehicles powered by electricity relatively limited works report the recycle of spent graphite (SG) anode
will account for more than 20 % of all vehicles. Lithium–ion batteries (Schiavi et al., 2021a,b).
(LIBs) are the power source for electric vehicles, from this point of view, Due to the high cost of existing remediation schemes, the industries
the development of LIBs will climb to another peak in the near future do not pay much attention to the recovery of spent lithium–ion battery
(Chen et al., 2020). Graphite is widely accepted as an ideal anode ma­ graphite anodes, which are generally used as a reducing agent to recover
terial for LIBs due to its excellent cycling stability and rate capability. As valuable metals or directly burned at high temperatures to collect the
estimated, graphite anode occupies over 15 % of the total mass and over copper. In contrast, several schemes have been proposed to recover
10 % of the manufacturing cost in commercial LIBs, demonstrating its spent lithium–ion battery graphite anodes within the laboratory context,
critical role (Alamerew and Brissaud, 2020; Alfaro–Algaba and Ram­ such as deionized water and hydrochloric acid washing to purify SG
irez, 2020; Arshad et al., 2020). As a matter of fact, as surveyed in 2021, (Wang et al., 2019; Yang et al., 2019), electrochemical electrolysis and
nearly 83 % of graphite anode for LIBs belonged to artificial graphite, microwave heating to strip SG (Cao et al., 2021; Chao et al., 2022), and
and the production of massive artificial graphite consumed a large high–temperature graphitization to repair graphite structures (Yu et al.,
number of petroleum resources, which undoubtedly exacerbates the 2021; Chen et al., 2022b). These schemes are not well targeted and often
energy and environment issues. cause significant energy consumption during the repair process,
Recently, a promising scheme of “LIBs repair & regeneration” has reducing the feasibility of recovery.

* Corresponding authors.
E-mail addresses: [email protected] (L. Yang), [email protected] (L. Chen).

https://doi.org/10.1016/j.resconrec.2023.107326
Received 7 March 2023; Received in revised form 15 September 2023; Accepted 18 November 2023
Available online 28 November 2023
0921-3449/© 2023 Elsevier B.V. All rights reserved.
K. Chen et al. Resources, Conservation & Recycling 201 (2024) 107326

In this work, we conducted systematical characterization and anal­ 2.4. Electrochemical tests
ysis on the failure of SG, and uncovered the related failure characteristic.
It was found that the failure of SG mostly results from the existence of The electrochemical properties of the samples were evaluated via the
high content impurities and damage of surface coating layer. Hereby, a two–electrode CR2025 coin cells, which are assembled in an argon–fil­
targeted repair scheme was put forward, which fully considers the led glove box (H2O < 1 ppm, O2 < 0.1 ppm). All of the electrodes were
combination of deep impurity removal and effective coating repair. The prepared by mixing 80 wt.% of active material, 10 wt.% polyvinylidene
results showed that the repaired graphite anode impurity residues fluoride, and 10 wt.% Super P evenly in N–methylpyrrolidone. Then, a
complied with the requirements of relevant National Standard (China copper foil was coated with a homogeneous slurry and dried at 60 ℃ in a
Lithium–ion Battery Graphite Anode Materials GB/T 24,533–2009, vacuum oven for 8 h. And use lithium foil and microporous poly­
hereby abbreviated as “CLBGAM”) and the broken cladding layer was propylene membrane as counter electrode and separator. The size of
effectively repaired. It was tested to show electrochemical performance each electrode was controlled as a circular disk with an average diam­
comparable to that of commercial graphite (CG) anodes. And the pro­ eter of 12 mm, and the mass loading of active material on each electrode
posed targeted repair scheme consumes 79 % less energy and reduces was set as ~1.2 mg cm–2. The electrolyte used in this work was made of
harmful emissions by 90 % when compared to existing repair solutions. LiPF6 (1M) dissolved into a mixed solvent of ethylene carbonate,
dimethylcarbonate and ethylmethyl carbonate (1:1:1 by volume). Gal­
2. Experimental vanostatic charge/discharge measurement was conducted on a multi­
channel battery testing system (CT2001A, China) between 0.01 and 3.0
2.1. Impurity removal of SG V (vs. Li+/Li). Cyclic voltammetry (CV) was carried out on an electro­
chemical workstation (CHI 760E, China). CV was taken at various scan
The detail of chemicals and materials can be found in the Supple­ rates 0.5 mV s− 1 within the same potential range from 0.01 to 3.0 V (vs.
mentary Material. Firstly, the spent battery anode was treated with Li+/Li). Electrochemical impedance spectroscopy (EIS) plots were
deionized water under ultrasonic condition followed by filtering and recorded on the open circuit potential within the frequency range from
drying to exfoliate SG from copper foil. In the following step, two 100 kHz to 0.01 Hz.
different impurity removal strategies were used in our work. One is
high–temperature annealing followed by acid leaching. Specifically, the 3. Results and discussion
exfoliated SG was firstly annealed at 530 ◦ C in air, and then leached by
2M HCl solution for 6 h at room temperature. The purified graphite 3.1. Failure characteristic analysis of SG
denoted as PG–1 could be obtained. The other strategy adopts a
completely reverse procedure, that is acid leaching followed by high­ It is widely acknowledged that the structure and composition of
–temperature annealing. The exfoliated SG was firstly leached by 2M graphite anode greatly determine the battery performance. When
HCl solution for 6 h at room temperature, and then filtered and annealed exploring the possible failure characteristic in SG, the content of residual
at 530 ℃ in air to acquire the final product marked as PG–2. impurities and the integrity of graphite layered structure as well as
surface coating layer should be simultaneously considered. With regard
2.2. Coating repair of PG to the influence of residual impurities, high content of metal impurities
(such as Fe and Cu) may pierce the separator and cause a short circuit,
Firstly, pitch (products derived from petroleum refining) was mixed while the existence of organic impurities (such as electrolyte and binder)
with the obtained PG–1 in a weight percentage of 8 wt.% with the assist will lead to serious graphite agglomeration and thus affect granulation.
of CS2 solvent. The concentration of PG–1 powder in CS2 solvent was In the meantime, the damage of graphite layered structure and surface
controlled to be ~0.04 g mL–1. After stirred for 20 mins at room tem­ coating layer is harmful to structure stability and will result in severe
perature, the resultant suspension was heated at 40 ◦ C to complete the capacity fading. Herein, to characterize and analyze the mentioned
evaporation of CS2. Subsequently, the PG–1/pitch mixture was further three factors, the inductive coupled plasma emission spectrometer (ICP),
annealed at 900 ◦ C for 3 h at a ramp rate of 10 ◦ C min–1 in Ar to convert thermogravimetric analysis (TGA), X–ray photoelectron spectroscopy
pitch into soft carbon layer, which accomplishes coating repair of PG (XPS), X–ray diffraction (XRD) and other techniques were all employed
and produces core–shell PG–CR–8 wt.% sample. For comparison, the to detect the structure and composition of SG.
pitch was also blended with PG–1 in a weight percentage of 3, 5 and 10 Fig. 2a shows the ICP result of SG. Clearly, series of different metal
wt.% by similar method, and the corresponding products were labelled impurities (including Al, Cu, Fe, Na etc.) can be witnessed, and the
as PG–CR–3 wt.%, PG–CR–5 wt.% and PG–CR–10 wt.%, respectively. contents of these metal impurities are far from satisfying the re­
quirements of CLBGAM (Al, Cu, Na etc. ≤ 5 ppm). Among them, Al, Cu
2.3. Material characterizations and Fe mostly come from the cathode and anode current collectors (Al
foil and Cu foil) and cathode active material (LiFePO4) respectively,
Inductive coupled plasma emission spectrometer (ICP, OPTIMA while Na mainly originates from the employed binder, i.e. carboxy­
8300, Thermo Scientific, USA) was used to analyze the removal effi­ methylcellulose sodium (CMC). Fig. 2b presents the TGA curves of SG in
ciency of metal impurities in SG. The thermal stability of SG was tested air and N2 atmospheres. Two obvious platforms can be found in the TGA
by thermogravimetric analysis (TGA, Diamond TG, Japan). X–ray curve tested in air. The weight loss before 530 ℃ is estimated to be ~7
photoelectron spectroscopy (XPS, Kratos AXIS Ultra DLD, UK) and wt.%, which corresponds to the volatilization of adsorbed water and
scanning electron microscope (SEM, JEOL JSM 7401, Japan) were used organic components. By contrast, the weight loss between 530 and 750
to analyze the impurity removal effect of PG and the repair effect of ℃ is ~93 wt.%, which is mainly caused by the oxidation of graphite.
PG–CR. X–ray diffraction (XRD, D 8 Advance, Bruker, Germany) was Clearly, these results are consistent with the TGA analysis tested in N2
employed to detect the graphitization degree of different carbon sam­ atmosphere (~7 wt.% weight loss). Fig. 2c presents high–resolution C 1
ples. Raman spectra (Raman, Renishaw inVia, UK) was utilized to s XPS spectra of SG, which can be fitted into four configurations: C=C
explore the disorder degree of different carbon samples. The damage (284.8 eV), C–C (285.1 eV), C–O (286.2 eV), –COOR (290.4 eV) (Li et al.,
status of surface coating layer in SG was analyzed by transmission 2019; Yi et al., 2022). The appearance of C–O and –COOR indicates the
electron microscope (TEM, TalosF200X, USA). presence of a certain amount of organic impurities in SG, which may
come from CMC and carbonate ester electrolyte (Han et al., 2022; Gu
et al., 2022; Chen et al., 2022a). The ICP, TGA and XPS results reveal the
existence of a certain amount of metal and organic impurities, and the

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net content of graphite in SG is far from meeting the demand of CLBGAM consumption, as shown in Fig. 1.
standard (≥ 99.7 %). The contents of residual metal impurities in PG–1 and PG–2 and the
The damage of graphite layered structure can be quantitatively corresponding impurity removal efficiency are displayed in Fig. 3a and
analyzed by the graphitization degree (P value) and disorder degree (ID/ S2. It can be seen from Fig. 3a that the metal impurity removal efficiency
IG value). The graphitization degree (P value) can be calculated by Eqs. of PG–1 is much higher than that of PG–2, and the metal impurity res­
(1) and (2), and the disorder degree (ID/IG value) can be estimated by the idues in PG–1 well meet the requirements of CLBGAM standard (Al, Cu,
intensity ratio of D band (~1350 cm–1) to G band (~1580 cm–1) from Na etc.≤ 5 ppm). The higher metal impurity removal efficiency for PG–1
Raman spectra (Yan et al., 2022). Combining the XRD patterns in Fig. 2d can be elucidated as follows. On one hand, the residual metal impurities
and Eqs. 1 and 2, we figured out that the P value of SG is 97.6 %, which is in SG can be converted to the corresponding metal oxides, which makes
nearly close to that of commercial graphite (P ≥ 95 %), well meeting the the removal of metal impurities more easily by subsequent acid leach­
CLBGAM (P ≥ 85 %) standard (Li et al., 2022b). The Raman spectra in ing. In addition, the organic components (such as CMC binder) in SG can
Fig. 2 g exhibit that the ID/IG value of SG is 0.15, which is close to that of be effectively removed in the first annealing step, which weakens the
CG (0.12) (Thambiliyagodage et al., 2018; Chen et al., 2018). The adsorption of metal impurities. As seen from the SEM images in Fig. 3e
interplanar spacing of SG is also consistent with that of CG, as seen from and f, almost no impurity can be found on the surface of PG–1 (the
the high–resolution transmission electron microscope (HRTEM) images absence of Na element was further confirmed by the mapping analysis in
in Fig. 2h and i. As reflected from the XRD, Raman and HRTEM results, it Fig. S1b), but some residues still can be observed on the surface of PG–2.
can be found that the layered structure of SG was not seriously damaged. The TGA curve in Fig. 3b shows no obvious multi–step platforms, indi­
cating complete removal of organic impurities in PG–1, which is
2d002 sinθ = nλ (1)
accorded with the SEM analysis. Additionally, the net content of
0.344 − d002 graphite in PG–1 is larger than 99.5 %, which is extremely close to the
P= × 100% (2) requirement of CLBGAM standard.
0.344 − 0.3354
Fig. 3c–d present the XRD patterns and Raman spectra of different
In general, during the manufacturing process of graphite anode, the samples. Apparently, the diffraction band at ~26.3◦ of PG–1 is sharper
graphite surface is suggested to be coated by an amorphous soft carbon than that of PG–2, indicating higher crystallinity of PG–1. The ID/IG
layer, which can be produced by thermal annealing pitch or phenolic value decreases from 0.15 for SG to 0.01 for PG–1 and 0.05 for PG–2,
resin. As a result, a typical core–shell graphite@soft carbon layer respectively, manifesting much reduced defect degree after impurity
structure can be formed before its practical application in LIBs (Li et al., removal. Compared to PG–2, the higher crystallinity and lower defect
2016; Hu et al., al.,2008; Dang et al., 2017; Liu et al., 2023). The degree for PG–1 indicate better purification effect. Therefore, the PG–1
as–formed core–shell structure is beneficial to preventing sample was selected to conduct the subsequent coating repair work.
co–intercalation of Li+ and organic solvent into graphite during char­
ge/discharge of LIBs. Fig. 2e and f show the scanning electron micro­ 3.2.2. Coating repair of PG
scope (SEM) images of CG and SG. It can be observed that the surface of After effective purification of SG, the following step is coating repair
CG is smooth and free of impurity, while the surface of SG is rough. of PG. Fig. 4a shows the repairing mechanism on PG–1. Specifically, the
Meanwhile, we found that SG agglomerates seriously, which is mostly pitch was firstly dissolved into CS2 solvent and then mixed with PG–1 to
due to the existence of residual organic impurities, such as CMC binder cover the damaged coating of PG–1. After high–temperature annealing,
(Na residues were found on the surface of SG, as shown in Fig. S1a). In the coated pitch was converted to soft carbon layer, which realizes the
addition to this, the HRTEM images in Fig. 2h and i show that uniform repair of damaged coating.
amorphous carbon coating layer appears on the surface of CG, while this Fig. 4b depicts the high–resolution C 1 s XPS spectra of SG, PG–1 and
coating layer on the surface on SG was broken and partially damaged, PG–CR. Compared to SG, the –COOR in PG–1 is disappearing and the
which is probably related to the uneven internal stress inside graphite C–O in PG–1 becomes much decreased, again demonstrating more
induced by the insertion and extraction of Li+ during long–term char­ efficient impurity removal. As reflected from Fig. 4c, the carbon content
ge/discharge process. The damage of graphite coating layer will un­ in PG–CR samples is growing with the increase of added pitch dosage.
doubtedly bring about the co–intercalation of Li+and organic solvent Meanwhile, it was evidenced from Fig. 4d that the percentage of C = O
into graphite structure, and further give rise to deteriorated battery (294.1 eV) in PG–CR samples also increases with the growing of added
performance (Park et al., 2009; Ohta et al., 2009). From this point of pitch (Hou et al., 2017; Xie et al., 2021). The increased C = O in PG–CR
view, the coating of SG should be well repaired to guarantee a satis­ samples is mostly concerned with the coated soft carbon layer derived
factory battery performance. from pitch.
As characterized and analyzed above, it can be witnessed that the The XRD patterns in Fig.3c and 5a show that the graphite layered
graphite layered structure of SG was not seriously damaged, and the structure was not significantly altered, as indicated from the almost
main reasons for the failure of SG are mostly correlated to the presence unchanged d002 value. The Raman spectra in Fig. 5b exhibits that the ID/
of high content impurities and damage of graphite coating layer. In this IG value gradually ascends from 0.01 for PG–1 to 0.11 for PG–CR–3 wt.
regard, a corresponding targeted repair scheme is put forward in the %, 0.16 for PG–CR–5 wt.%, 0.23 for PG–CR–8 wt.% and 0.32 for
following. PG–CR–10 wt.%, respectively, implying enhanced defect degree. The
XPS spectra of SG; (d) XRD patterns of SG and CG; (e–f) SEM images gradual enhanced defect degree can be attributable to the increased
of SG and CG; (g) Raman spectra of SG and CG; (h–i) HRTEM images of amorphous carbon layer derived from pitch. As displayed in the SEM
SG and CG and transmission electron microscope (TEM) images in Fig. 5c–f, the
surfaces of PG–CR–3 wt.% and PG–CR–5 wt.% are not that smooth due
3.2. Targeted repair of SG to the introduction of limited pitch, which further leads to the formation
of incomplete carbon layer (Ma et al., 2022; Sun et al., 2022). With
3.2.1. Purification of SG respect to PG–CR–8 wt.% sample, its surface is proven to be much
The repair of coating for SG anode resembles the repair of wound for smooth, indicating the generation of relatively intact coating layer
human beings. It is always suggested to clean the wound before suturing (Fig. 5e and S4). While for PG–CR–10 wt.%, its surface appears uneven
the wound. Likewise, it is essential to purify SG prior to repairing the and partially damaged, which can be ascribed to the fact that over–thick
coating of SG. In our work, two purification strategies (annealing + acid amorphous carbon derived from excessive pitch brings about the
leaching and acid leaching + annealing) were proposed to pursue better structure collapse of coating layer during subsequent ball–milling pro­
Contaminant removal results with the same energy and drug cess. Clearly, all these results imply that PG–CR–8 wt.% sample achieves

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K. Chen et al. Resources, Conservation & Recycling 201 (2024) 107326

Fig. 1. Flowchart of SG repair process.

Fig. 2. (a) ICP result of SG; (b) TGA curves of SG in air and N2 atmosphere; (c) C 1 s.

the most effective coating repair effect. Obviously, the above analysis peak at ~0.2 V and a broad peak between 0.3~1.0 V in the first cycle
shows that 8 wt.% of pitch can efficiently repair the broken graphite (Liu et al., 2022; Wang et al., 2020), which correspond to the Li+
coating. intercalation process and the formation of solid electrolyte interphase
(SEI) film (Li et al., 2022a). It was found from Fig. S5 that the CV curves
3.3. Electrochemical performance of CG electrode exhibit analogous redox peaks to those of PG–CR–8 wt.%
electrode, implying similar electrochemical process. The charge/di­
Herein, we employed PG–CR–8 wt.% sample as the anode for LIBs, scharge profiles of PG–CR–8 wt.% electrode in Fig. 6b show an obvious
and tested its electrochemical performance by cyclic voltammetry (CV), platform at ~0.2 V and an inconspicuous platform at ~0.8 V, which are
galvanostatic charge/discharge (GCD) and electrochemical impedance assigned to the Li+ insertion and formation of SEI film, respectively
spectra (EIS) techniques (Yang et al., 2023a,b). As seen from the CV (Heiskanen et al., 2019; Louli et al., 2019). Apparently, this result is in
curves in Fig. 6a, the PG–CR–8 wt.% electrode displays a prominent good agreement with the CV analysis.

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K. Chen et al. Resources, Conservation & Recycling 201 (2024) 107326

Fig. 3. (a) ICP results of PG–1 and PG–2; (b) TGA curves of PG–1 in air and N2 atmosphere; (c) XRD patterns of PG–1 and PG–2; (d) Raman spectra of PG–1 and PG–2;
(e–f) SEM images of PG–1 and PG–2.

Fig. 6c presents the cycling performance of SG, PG–CR–8 wt.% and To further investigate the electrochemical properties of PG–CR–8 wt.
CG electrodes at the current density of 1 C (372 mA g–1). The specific % electrode, the EIS technique was also used. Fig. 6e shows the EIS plots
capacity of SG electrode is far inferior to that of CG electrode, and the of SG, PG–CR–8 wt.% and CG electrodes, and the corresponding
specific capacity value suffers from a significant decline after 300 cycles. equivalent circuit fitting results are listed in Table S1. It can be discerned
The unsatisfactory cycling performance for SG electrode is mostly from Fig. 6e that all EIS plots contain a semicircle in high–frequency
correlated to the existence of impurities and the damage of graphite region and an inclined straight line in low–frequency region (Han et al.,
coating layer. On one hand, the existing impurities occupy the volume al.,2018; Lai et al., 2018). In general, the diameter of the semicircle in
and weight of the anode material, which undoubtedly lowers the specific high–frequency region represents the charge transfer resistance (RCT),
mass capacity. At the same time, the damage of graphite coating layer and the straight line in low–frequency region reflects the Warburg
will cause the co–insertion of Li+and organic solvent, which further impedance associated with Li+ diffusion inside the entire electrode (Son
results in deteriorated cycling stability. By contrast, our prepared et al., 2020; Gent et al., 2022; Tu et al., 2022). Based on Table S1, the RCT
PG–CR–8 wt.% electrode displays higher specific capacity and much value (108.1 Ω) of PG–CR–8 wt.% electrode is smaller than that (137.0
better cycling stability when compared to SG. After continuous 450 Ω) of SG electrode, indicating promoted charge transfer kinetics.
cycles, the specific capacity of PG–CR–8 wt.% electrode still delivers a Meanwhile, the slope of straight line for PG–CR–8 wt.% electrode is
specific capacity as high as 355 mAh g–1 along with a high coulombic proven to be larger than that for SG electrode, demonstrating faster
efficiency of over 98 %, which is much approaching to that for CG Li+diffusion rate. Fig. 6f displays the EIS plots of PG–CR–8 wt.% elec­
electrode, demonstrating outstanding cycling stability. trode before and after cycling for different cycles. It was evidenced that
Fig. 6d exhibits the rate performance of the three electrodes. It can be the RCT value gradually declines with the increase of cycle number from
clearly witnessed that the PG–CR–8 wt.% electrode delivers a stable one to ten cycles, suggesting improved electrochemical kinetics, which
discharge capacity of 347 mAh g–1 at 0.1 C, and this value still keeps as is mostly related to the gradual activation of PG–CR–8 wt.% electrode
250 mAh g–1 at a high current density of 2 C. When the current density during charge/discharge process.
gets back to 0.1 C, the discharge capacity returns to 347 mAh g–1. By
comparison, the discharge capacities of PG–CR–8 wt.% electrode is 3.4. Economic and environmental analysis
higher than those of SG, and prove close to those of CG at all set current
densities, verifying much better rate capability. Compared to SG elec­ The economic and environmental protection index should be
trode, this enhanced rate performance for PG–CR–8 wt.% electrode is considered for the practical application of any “LIBs repair & regener­
mainly due to deep removal of impurities and effective repair of coating ation” scheme. Usually, the disposal strategy for spent battery anodes in
layer. most enterprises is just selling the stripped copper foil (partial recovery).

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K. Chen et al. Resources, Conservation & Recycling 201 (2024) 107326

Fig. 4. (a) Schematic diagram of repairing mechanism on PG–1; (b) High–resolution C 1 s XPS spectra and (c–d) Surface element and functional group contents of
different samples.

Fig. 5. (a) XRD patterns of PG–CR samples; (b) Raman spectra of PG–CR samples; (c–f) SEM images of PG–CR samples.

Previously reported repair schemes often consume large amounts of the Greenhouse Gas, Regulated Emissions, and Energy Use in Trans­
energy for graphitization, which not only reduces the economic benefits portation (GREET) model (Argonne National laboratory, 2022) was used
of recycling, but becomes a heavy burden on the environment. Herein, to analyze the economic and environmental assessment of this program

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K. Chen et al. Resources, Conservation & Recycling 201 (2024) 107326

Fig. 6. (a) CV curves for the initial three cycles and (b) Charge/discharge profiles of PG–CR–8 wt.% electrode; (c) Cycling performance of CG, SG, PG–CR–8 wt.%
electrodes at 1 C; (d) Rate performance of CG, SG, PG–CR–8 wt.% electrodes at different current densities; (e) Nyquist plots of different electrodes before cycling; (f)
Nyquist plots of PG–CR–8 wt.% electrode before and after cycling for different cycles.

(detailed calculations are shown in Table S2–4). Fig. 7 shows the life value. Undoubtedly, our work not only provides an effective solution to
cycle analysis of the targeted repair, graphitization and partial recovery reduce the pressure from environmental protection and resource usage,
methods. It can be seen that the targeted repair scheme proposed in this but offers a possibility to make a profit by purifying and repairing SG.
work is highly targeted to avoid the high temperature graphitization
step, so it seems much better than those currently used by companies or 4. Conclusion
reported by previous works from the perspective of economics and
pollutant emissions. Compared to the high–temperature graphitization In summary, a systematic characterization and analysis of the
repair scheme used in previous works, the targeted repair scheme pro­ structure and composition of SG was performed in order to perform an
posed in this work consumes 79 % less energy and reduces emissions of accurate repair. It is confirmed that the failure of SG mostly originates
CO2 by up to 80 % and SOx, NOx by up to 85 % and 75 %. In terms of from the existence of high content impurities and damage of surface
energy consumption, pollutant emissions, and economic benefits, it is coating layer. Accordingly, the relevant repair scheme combining im­
substantially better than the direct incineration scheme for copper re­ purity removal and coating repair is put forward. The results show that
covery currently used by companies. In spite of the whole estimation at a our proposed repair scheme achieves deep removal of impurities and
lab level, we believe the actual industrial profit will be far more than this effective repair of coating layer, and the quality of the obtained purified

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K. Chen et al. Resources, Conservation & Recycling 201 (2024) 107326

Fig. 7. (a) Life cycle analysis of targeted repair, graphitization and partial recovery methods; (b) GHG emissions analysis; (c) Atmospheric pollutants analysis; (d)
Radar plot comparing various characteristics of targeted repair, graphitization and partial recovery methods.

graphite after coating repair (PG–CR–8 wt.%, 8 wt.% represents the editing, Supervision, Project administration, Funding acquisition.
mass ratio of pitch to purified graphite) well meet the relevant National
Standard (China Lithium–ion Battery Graphite Anode Materials GB/T
Declaration of Competing Interest
24533–2009). In addition, the electrochemical performance of
PG–CR–8 wt.% electrode is proven to be significantly promoted when
The authors declare that they have no known competing financial
compared to SG. The specific capacity of PG–CR–8 wt.% electrode rea­
interests or personal relationships that could have appeared to influence
ches as high as 355 mAh g–1 after 450 cycles at a current density of 1 C
the work reported in this paper.
along with a high coulombic efficiency of over 98 %, and this value still
retains as 250 mAh g–1 at a high current density of 2 C. The proposed
Data availability
targeted repair scheme is also evaluated to reduce energy consumption
by 79 % and harmful pollutants emitted by 90 %. Compared with the
No data was used for the research described in the article.
incineration and recovery of copper solution commonly used by com­
panies today, it has obvious advantages in terms of both energy con­
sumption and harmful gas emissions as well as economic benefits.
Obviously, our work can be a guide to provide a feasible solution for the Acknowledgements
recovery of graphite anodes from spent LIBs by understanding the fail­
ure characteristics of graphite anodes. This work was financially supported by the Key Project of Research
and Development Plan of Jiangxi Province (No. 20223BBG74006 and
20201BBE51007), Natural Science Foundation of Hunan Province (No.
Data availability
2023JJ30277), the Science & Technology Talents Lifting Project of
Hunan Province (No. 2022TJ‒N16), the Scientific Research Fund of
Data will be made available on request.
Hunan Provincial Education Department, China (No. 21A0392).

CRediT authorship contribution statement Supplementary materials

Kechun Chen: Conceptualization, Data curation, Writing – original Supplementary material associated with this article can be found, in
draft. Yuan Ding: Methodology. Liming Yang: Writing – review & the online version, at doi:10.1016/j.resconrec.2023.107326.
editing, Supervision, Project administration, Funding acquisition. Zhi­
hao Wang: Investigation. Haoxuan Yu: Investigation. Difan Fang:
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