Recycling of Graphite Anode from Spent Lithium‐ion Batteries for Preparing Fe‐N‐doped Carbon ORR Catalyst

Ruan, Dingshan; Zou, Ke; Du, Ke; Wang, Fengmei; Wu, Lin; Zhang, Zhenhua; Wu, Xiaofeng; Hu, Guorong

doi:10.1002/cctc.202001867

Cited by 26 publications

(18 citation statements)

References 45 publications

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“…Simultaneously, the impurity in spent graphite will be removed. Ruan et al [137] synthesized an ORR catalyst (Figure 9c) by pyrolyzing spent graphite with polyaniline, and iron salt. The spent graphite acts as a carbon carrier, meanwhile, residual transition metals can promote the catalytic activity.…”

Section: Recovery Of Anode and Electrolytementioning

confidence: 99%

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Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries

Wu¹,

Xu²

2022

MatLab

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Lithium-ion batteries (LIBs), as the advanced power batteries with comprehensive performance, have widely used in electric vehicles (EVs), military equipment, aerospace, consumer electronics, and other fields. With the surge in demand for LIBs, the number of spent LIBs has increased rapidly. However, if the spent LIBs just are simply landfilled, the hazardous components contained in them such as heavy metals and organic electrolytes will pollute the environment, and ultimately threaten human health. In addition, some valuable components will be wasted by landfill, especially high-value metal elements contained in cathode. Thus, the recycling of spent LIBs is a “two birds with one stone” strategy which is not only beneficial to environmental protection but also has high economic value. Accordingly, great efforts have been made to develop efficient and cost-effective recycling processes for spent LIBs recovery. In line with the recycling process, this review first presents a series of pretreatment progresses (disassembling, inactivation, dismantling, and separation) and discusses the problems and challenges involved (automation, environmental protection, and cost, etc.). Second, we summarize and discuss the current recovery and regeneration technologies for cathode materials, including pyrometallurgy, hydrometallurgy and electrochemistry. In addition, advances in the recovery of anode and electrolyte are also introduced. Finally, based on the current state of recycling, we cautiously make some suggestions and prospects for the future recycling of spent LIBs, with a view to providing more ideas for the recycling of used LIBs.

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Section: Recovery Of Anode and Electrolytementioning

confidence: 99%

mentioning

confidence: 99%

Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries

Wu¹,

Xu²

2022

MatLab

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“…[36] Among these nitrogen species, pyridinic N can significantly contribute to ORR performance by weakening the OÀ O bond, while graphitic N enhances the conductivity of the catalyst. [37] In the same scenario, S 2p spectra also show four characteristic peaks of MÀ S, CÀ S, C=S, and SÀ O x at 162.09, 163.98, 165.87, and 168.41 eV. [35,38] In addition, the structural characteristic of surface oxygen atoms (O 1s) exhibits four characteristic peaks of lattice O atoms at 529.5, 531.08, 531.9, and 534.5 eV corresponding to MÀ OÀ M, C=O, CÀ OÀ C/CÀ OH, and OÀ S. [39] Consequently, the results illustrate the successful preparation of N and S atoms in FeCoÀ N,S@CNFs, resulting in the introduction of N and S atoms.…”

Section: Structural and Compositional Characterization Of Feco-ns@cnfsmentioning

confidence: 99%

N,S‐co‐doped FeCo Nanoparticles Supported on Porous Carbon Nanofibers as Efficient and Durable Oxygen Reduction Catalysts

et al. 2022

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Finding high-performance, low-cost, efficient catalysts for oxygen reduction reactions (ORR) is essential for sustainable energy conversion systems. Herein, highly efficient and durable iron (Fe) and cobalt (Co)-supported nitrogen (N) and sulfur (S) codoped three-dimensional carbon nanofibers (FeCoÀ N, S@CNFs) were synthesized via electrospinning followed by carbonization. The as-prepared FeCoÀ N,S@CNFs served as efficient ORR catalysts in alkaline 0.1 m KOH solutions that were N 2 and O 2saturated.The experimental results revealed that FeCoÀ N,S@CNFs were highly active ORR catalysts with defectrich active pyridinic N and pyrrolic N and metal bonds to N and S atom sites, which enhanced the ORR activity. FeCoÀ N,S@CNFs exhibited a high onset potential (E onset = 0.89 V) and half-wave potential (E 1/2 = 0.85 V), similar to the electrocatalytic activity of commercial Pt/C. Additionally, the durability of the as-prepared FeCoÀ N,S@CNFs catalysts was maintained for 14 h with longterm stability and high tolerance to methanol stability, accounting for their excellent catalytic ability. Furthermore, CoÀ N@CNFs, FeÀ N@CNFs, and varying Fe and Co ratios were compared with those of FeCoÀ

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“…However, if spent graphite anode is directly used as the regeneration anode material of LIBs, which inevitably causes metal impurities to react with the electrolyte and generate fluoride salts, specific problems such as the reduction of the first-cycle coulomb efficiency and excessive consumption of the electrolyte are bound to arise. − Therefore, purification must be conducted before regeneration . Traditionally, chemical and physical purification methods are the main techniques for graphite production.…”

Section: Introductionmentioning

confidence: 99%

A Novel Low-Temperature Fluorination Roasting Mechanism Investigation of Regenerated Spent Anode Graphite via TG-IR Analysis and Kinetic Modeling

et al. 2022

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Spent anode graphite, a hazardous solid waste discarded from the recovery of spent lithium-ion batteries (LIBs), had created social and environmental issues but has been scarcely investigated. Thus, a feasible, environmentally friendly, and economical process of low-temperature fluorination roasting and water leaching technology was proposed to regenerate spent graphite anodes. The results showed that the physical and chemical properties of regenerated graphite with a purity of 99.98% reached the graphite anode standard of LIBs and exhibited a stable specific capacity (340.9 mAh/g), capacity retention (68.92% after 470th cycles), and high initial Coulombic efficiency (92.13%), much better than that of waste carbon residue and similar to that of commercial graphite. Then the reaction mechanism and kinetic modeling of fluorination roasting of spent anode material was mainly explored by differential thermogravimetry and nonisothermal analysis methods. The results showed that the complexation and phase-transformation process of non-carbon valuable components in spent anode graphite occurred through three consecutive reactions in the 80–211 °C temperature intervals. The reaction mechanism of the whole process can be kinetically characterized by three successive reactions: third-order chemical reaction, Z-L-T eq, and second-order chemical reaction. Moreover, the thermodynamic functions of the fluorination roasting were calculated by the activated complex theory (transition state), which indicated the process was nonspontaneous. The mechanistic information was in good agreement with thermogravimetric-infrared spectroscopy (TG-IR), electron probe microanalysis, scanning electron microscopy, energy-dispersive spectrometry, and simulation experiments results.

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Recycling of Graphite Anode from Spent Lithium‐ion Batteries for Preparing Fe‐N‐doped Carbon ORR Catalyst

Cited by 26 publications

References 45 publications

Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries

Advances and Challenges on Recycling the Electrode and Electrolyte Materials in Spent Lithium-Ion Batteries

N,S‐co‐doped FeCo Nanoparticles Supported on Porous Carbon Nanofibers as Efficient and Durable Oxygen Reduction Catalysts

A Novel Low-Temperature Fluorination Roasting Mechanism Investigation of Regenerated Spent Anode Graphite via TG-IR Analysis and Kinetic Modeling

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