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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 Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 64030:Environmental materials and recycle technology-related
Research InstitutionTohoku University

Principal Investigator

ZHENG QINGXIN  東北大学, 工学研究科, 特任助教 (30835509)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2023: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2022: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2021: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000)
KeywordsRecycling / Lithium-ion batteries / Hydrothermal leaching / Metal recovery / Acid corrosion / Glycine / Citric acid / Mixed organic acid / Mixed organic acids / Continuous / Kinetic study / Metal isolation / Mn isolation / Continuous leaching / Unreacted core model / Organic acid
Outline of Research at the Start

Metal recovery from spent lithium-ion batteries (LIBs) is an increasingly urgent topic in the world. Hydrometallurgy is the most common and industrially adopted method of metal recovery and comprises two steps of leaching and separation. Here, the applicant aims to explore an organic acid (amino acid or mixed organic acids) to achieve the efficient hydrothermal leaching of spent LIBs with low or no acid corrosion. The elimination of acid corrosion is supposed to greatly develop the method of hydrothermal leaching, improve the current leaching process, and further promote hydrometallurgy.

Outline of Final Research Achievements

In this project, the Principal Investigator aimed to explore a kind of organic acids for the hydrothermal leaching of spent lithium-ion battery (LIB) cathode materials, which can achieve high leaching efficiency and resolve the problem of acid corrosion. Based on a literature investigation and initial experiments, glycine and citric acid/glycine mixture were selected as candidate leaching agents. Finally, it was the first time to achieve the acid leaching of different types of LIB cathode materials including LiCoO2, LiNiO2, and LiMn2O4, and LiNixMnyCo1-x-yO2 (NCM), through a green process with high efficiency of about 100% and low/no acid corrosion.
During the research period, 4 peer-reviewed English papers were published in top journals such as ACS Sustainable Chemistry and Engineering, a patent was submitted, and six oral presentations and one poster presentation were delivered, including two invited presentations, at international and domestic conferences.

Academic Significance and Societal Importance of the Research Achievements

This research effectively eliminated the acid corrosion problem during the leaching process, significantly improving current LIB recycling methods. The results will help conserve natural resources, reduce environmental problems, ensure resource stability and security, and bring economic benefits.

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Research-status Report
  • 2021 Research-status Report
  • Research Products

    (13 results)

All 2023 2022 2021 Other

All Journal Article (4 results) (of which Peer Reviewed: 4 results,  Open Access: 1 results) Presentation (7 results) (of which Int'l Joint Research: 2 results,  Invited: 2 results) Remarks (1 results) Patent(Industrial Property Rights) (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 Issue: 35 Pages: 13033-13042

    • DOI

      10.1021/acssuschemeng.3c02854

    • Related Report
      2023 Annual Research Report
    • 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 Issue: 4 Pages: 2300421-2300421

    • DOI

      10.1002/adsu.202300421

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Metal Recovery of LiCoO2/LiNiO2 Cathode Materials by Hydrothermal Leaching and Precipitation Separation2022

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

      ACS Sustainable Chemistry & Engineering

      Volume: 10 Issue: 38 Pages: 12852-12863

    • DOI

      10.1021/acssuschemeng.2c04259

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Journal Article] Single-Step Recovery of Divalent Mn Component from LiMn2O4 Cathode Material at Hydrothermal Conditions as an Mn-Citrate Complex2021

    • Author(s)
      Zheng Qingxin、Shibazaki Kensuke、Ogawa Tetsufumi、Watanabe Masaru
    • Journal Title

      ACS Sustainable Chemistry & Engineering

      Volume: 9 Issue: 33 Pages: 10970-10976

    • DOI

      10.1021/acssuschemeng.1c03459

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [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
    • Related Report
      2023 Annual Research Report
    • 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
    • Related Report
      2023 Annual Research Report
  • [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
    • Related Report
      2023 Annual Research Report
  • [Presentation] Development of Hydrothermal Leaching Technology for Recycling of Spent Lithium-ion Batteries2023

    • Author(s)
      Qingxin Zheng、Masaru Watanabe
    • Organizer
      SCEJ 89th Annual Meeting
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] METAL RECOVERY OF THE LEACHATE OBTAINED FROM COMMERCIAL CATHODE MATERIALS BY HYDROTHERMAL LEACHING2022

    • Author(s)
      NAKAJIMA Akitoshi, ZHENG Qingxin, OGAWA Tetsufumi, NAKAYASU Yuta, WATANEBE Masaru
    • Organizer
      9th International Conference on Engineering for Waste and Biomass Valorisation (WasteEng2022)
    • Related Report
      2022 Research-status Report
  • [Presentation] LOW/NO-CORROSION LEACHING OF SPENT LITHIUM-ION BATTERY CATHODE MATERIALS BY HYDROTHERMAL METHOD USING AMINO ACID ORMIXED ORGANIC ACIDS AS THE LEACHANT2022

    • Author(s)
      ZHENG Qingxin, OGAWA Tetsufumi, NAKAJIMA Akitoshi, WATANABE Masaru
    • Organizer
      9th International Conference on Engineering for Waste and Biomass Valorisation (WasteEng2022)
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] Application of Hydrothermal Leaching Technology to Spent LIB Cathode Materials withCitric Acid Using Batch-type Device and Flow System2022

    • Author(s)
      ,Masaru Watanabe, Qingxin Zheng, Kensuke Shibazaki, Tetsufumi Ogawa, Atsushi Kishita, Yuya Hiraga
    • Organizer
      化学工学会 第53回秋季大会
    • Related Report
      2022 Research-status Report
    • Invited
  • [Remarks] https://researchmap.jp/Qingxin_Zheng

    • Related Report
      2023 Annual Research Report
  • [Patent(Industrial Property Rights)] クエン酸マンガンの製造方法2021

    • Inventor(s)
      渡邉 賢 , 鄭 慶新 , 宮崎 秀喜
    • Industrial Property Rights Holder
      国立大学法人東北大学 , 恵和興業株式会社
    • Industrial Property Rights Type
      特許
    • Patent Publication Number
      2022-169401
    • Filing Date
      2021
    • Related Report
      2022 Research-status Report

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Published: 2021-04-28   Modified: 2025-01-30  

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