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2023 Fiscal Year Annual Research Report

Low/no-corrosion leaching of spent lithium-ion battery cathode materials in hydrothermal water using amino acid or mixed organic acids as the leachant

Research Project

Project/Area Number 21K12302
Research InstitutionTohoku University

Principal Investigator

鄭 慶新  東北大学, 工学研究科, 特任助教 (30835509)

Project Period (FY) 2021-04-01 – 2024-03-31
KeywordsLithium-ion batteries / Hydrothermal leaching / Mixed organic acids / Continuous / Kinetic study / Metal isolation / Mn isolation
Outline of Annual Research Achievements

Hydrothermal leaching of spent LiNixCoyMn1-x-yO2 (NCM) and commercial LiMn2O4 (LMO) cathode materials was conducted by applying glycine as a leaching agent. With the increase in reaction temperature and time, the leaching efficiencies of Co, Ni, and Mn significantly increased, but even at 200 °C for 15 min, the leaching efficiency of Mn was as low as 16%. Compared with Li, Co, and Ni, the leaching performance of Mn was much poorer, but this special property makes it possible for glycine to isolate Mn directly from LMO cathode material.
During the hydrothermal leaching of commercial LMO cathode material with glycine, the leaching efficiency of Li significantly increased with reaction temperature and time, and was much higher than that of Mn under the same condition. The results of kinetic study revealed that the activation energy of Li leaching was much lower than that of Mn. At 200 °C for 120 min, the leaching efficiencies of Li and Mn achieved 99.5% and 7.6%, respectively, which means that 92.4% of Mn was successfully isolated and kept in the solid residue. After calcinating at 600 °C for 1h, the final product was obtained and identified to be Mn2O3 with a purity of 99.0%.
Furtheremore, the metal isolation of the leachates obtained from the hydrothermal leaching of commercial NCM cathode materials with mixed organic acids has been studied in depth. Mn was successfully precipitated by alkaline from the leachate in the first step, making it possible to realize the robotic arm-assisted continuous precipitation isolation of Mn, Co, Ni, and Li.

  • Research Products

    (7 results)

All 2023 Other

All Journal Article (2 results) (of which Peer Reviewed: 2 results,  Open Access: 1 results) Presentation (4 results) (of which Int'l Joint Research: 1 results,  Invited: 1 results) Remarks (1 results)

  • [Journal Article] Excellent Performance of Glycine in Isolating Mn during Hydrothermal Leaching of LiMn2O4 Cathode Materials2023

    • Author(s)
      Zheng Qingxin、Hirama Seiya、Nakajima Akitoshi、Ogawa Tetsufumi、Nakayasu Yuta、Li Zixian、Watanabe Masaru
    • Journal Title

      ACS Sustainable Chemistry & Engineering

      Volume: 11 Pages: 13033~13042

    • DOI

      10.1021/acssuschemeng.3c02854

    • Peer Reviewed
  • [Journal Article] Organic Acid‐Based Hydrothermal Leaching of LiFePO4 Cathode Materials2023

    • Author(s)
      Li Zixian、Zheng Qingxin、Nakajima Akitoshi、Zhang Zhengyang、Watanabe Masaru
    • Journal Title

      Advanced Sustainable Systems

      Volume: 8 Pages: 2300421

    • DOI

      10.1002/adsu.202300421

    • Peer Reviewed / Open Access
  • [Presentation] Metal recovery of LiMn2O4-based spent lithium-ion battery cathode material using hydrothermal leaching with organic acids and precipitation separation2023

    • Author(s)
      Masaru Watanabe、Qingxin Zheng、Akitoshi Nakajima
    • Organizer
      19th European Meeting on Supercritical fluids
    • Int'l Joint Research
  • [Presentation] Application of hydrothermal leaching process with organic acids on LiFePO4 cathode materials2023

    • Author(s)
      Zixian Li、Qingxin Zheng、Masaru Watanabe
    • Organizer
      化学系学協会東北大会
  • [Presentation] Hydrothermal leaching of LiFePO4 using organic acids2023

    • Author(s)
      李 子賢、鄭 慶新、渡邉 賢
    • Organizer
      化学工学会第54回秋季大会
  • [Presentation] Development of Hydrothermal Leaching Technology for Recycling of Spent Lithium-ion Batteries2023

    • Author(s)
      Qingxin Zheng、Masaru Watanabe
    • Organizer
      SCEJ 89th Annual Meeting
    • Invited
  • [Remarks] https://researchmap.jp/Qingxin_Zheng

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Published: 2024-12-25  

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