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Repurposing of Fruit Peel Waste as a Green Reductant for Recycling of Spent Lithium-Ion Batteries

  • Zhuoran Wu
    Zhuoran Wu
    Energy Research Institute, Nanyang Technological University, 50 Nanyang Drive, 637553 Singapore
    More by Zhuoran Wu
  • Tanto Soh
    Tanto Soh
    Energy Research Institute, Nanyang Technological University, 50 Nanyang Drive, 637553 Singapore
    More by Tanto Soh
  • Jun Jie Chan
    Jun Jie Chan
    Energy Research Institute, Nanyang Technological University, 50 Nanyang Drive, 637553 Singapore
    School of Materials Science and Engineering, Nanyang Technological University, Nanyang Avenue, 639798 Singapore
    More by Jun Jie Chan
  • Shize Meng
    Shize Meng
    School of Materials Science and Engineering, Nanyang Technological University, Nanyang Avenue, 639798 Singapore
    More by Shize Meng
  • Daniel Meyer
    Daniel Meyer
    Institut de Chimie Séparative de Marcoule (ICSM), UMR 5257 CEA−CNRS−UM−ENSCM, Centre de Marcoule, BP 17171, 30207 Bagnols-sur-Cèze Cedex, France
    More by Daniel Meyer
  • Madhavi Srinivasan*
    Madhavi Srinivasan
    Energy Research Institute, Nanyang Technological University, 50 Nanyang Drive, 637553 Singapore
    School of Materials Science and Engineering, Nanyang Technological University, Nanyang Avenue, 639798 Singapore
    *Email: [email protected]
  • , and 
  • Chor Yong Tay*
    Chor Yong Tay
    Energy Research Institute, Nanyang Technological University, 50 Nanyang Drive, 637553 Singapore
    School of Materials Science and Engineering, Nanyang Technological University, Nanyang Avenue, 639798 Singapore
    School of Biological Sciences, Nanyang Technological University, 60 Nanyang Drive, 637551 Singapore
    *Email: [email protected]
Cite this: Environ. Sci. Technol. 2020, 54, 15, 9681–9692
Publication Date (Web):July 9, 2020
https://doi.org/10.1021/acs.est.0c02873
Copyright © 2020 American Chemical Society

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    Abstract

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    The development of environmentally benign hydrometallurgical processes to treat spent lithium-ion batteries (LIBs) is a critical aspect of the electronic-waste circular economy. Herein, as an alternative to the highly explosive H2O2, discarded orange peel powder (OP) is valorized as a green reductant for the leaching of industrially produced LIBs scraps in citric acid (H3Cit) lixiviant. The reductive potential of the cellulose- and antioxidant-rich OP was validated using the 3,5-dinitrosalicylic acid and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic) acid assays. Leaching parameters such as OP concentration (200 mg), processing temperature (100 °C), H3Cit concentration (1.5 M), reaction duration (4 h), and slurry density (25 g/mL) were systematically optimized to achieve 80–99% leaching efficiencies of Ni, Mn, Co, and Li from the LIB “black mass”. Importantly, solid side-streams generated by the OP-enabled leaching displayed negligible cytotoxicity in three different human cell lines, suggesting that the process is environmentally safe. As a proof of concept, Co(OH)2 was selectively recovered from the green lixiviant and subsequently utilized to fabricate new batches of LiCoO2 (LCO) coin cell batteries. Galvanostatic charge–discharge test revealed that the regenerated batteries exhibited initial charge and discharge values of 120 and 103 mAh/g, respectively, which is comparable to the performance of commercial LCO batteries. The use of fruit peel waste to recover valuable metals from spent LIBs is an effective, ecofriendly, and sustainable strategy to minimize the environmental footprint of both waste types.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c02873.

    • Compositional analysis of orange peel (OP) (Table S1), SEM images of pure LCO and LIB black mass (Figure S1), X-ray fluorescence spectrum of the recovered cobalt hydroxide (Figure S2), and recovery efficiency of Co retrieved from four different batches of the OP leaching solution (Figure S3) (PDF)

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