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Development of novel recycling technology for rare earths combined wet separation and electrodeposition using ionic liquids

Research Project

Project/Area Number 24686101
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypePartial Multi-year Fund
Research Field Recycling engineering
Research InstitutionYokohama National University

Principal Investigator

MATSUMIYA Masahiko  横浜国立大学, 環境情報研究科(研究院), 准教授 (00370057)

Project Period (FY) 2012-04-01 – 2015-03-31
Project Status Completed (Fiscal Year 2014)
Budget Amount *help
¥8,060,000 (Direct Cost: ¥6,200,000、Indirect Cost: ¥1,860,000)
Fiscal Year 2014: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2013: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Fiscal Year 2012: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Keywords有価物回収 / イオン液体 / レアアース / リサイクル / イオン液体電析法 / 応用電気化学 / 環境電気化学
Outline of Final Research Achievements

In this study, we developed a novel recycling process of rare earth metals from Nd-Fe-B magnets, which was composed of the following steps: pretreatment, wet separation and electrodeposition using ionic liquids. The leaching ratio of Nd3+ and Fe3+ was 91.5% and 5.8%, respectively. Then, Fe(OH)3 precipitate was generated by adding Ca(OH)2 at pH~4.5 on deironization process. As a result, Fe(OH)3 was perfectly removed by solid-liquid separation and the separation factor of Fe was >99.9%. This result allowed us to demonstrate that the electrodeposition energy of residual Fe was 0 kJ/mol. The electrodeposition of Nd metal was performed in ionic liquids under potentiostatic condition of -3.25V at 393K. As for the Nd deposits, Nd metal layer at the depth of 0.62um was confirmed by XPS analysis. Finally, the total recovery energy of Nd-1t was estimated at 1.8MWh/t, which was extremely low compared with the conventional technology and we contributed to the development of energy-saving process.

Report

(4 results)
  • 2014 Annual Research Report   Final Research Report ( PDF )
  • 2013 Annual Research Report
  • 2012 Annual Research Report
  • Research Products

    (46 results)

All 2015 2014 2013 2012 Other

All Journal Article (17 results) (of which Peer Reviewed: 17 results,  Open Access: 5 results,  Acknowledgement Compliant: 3 results) Presentation (23 results) (of which Invited: 3 results) Remarks (3 results) Patent(Industrial Property Rights) (3 results)

  • [Journal Article] Self-diffusion behaviors of ionic liquids by MD simulation based on united-atom force field introduced charge scaling by ab initio MO simulation2015

    • Author(s)
      Masahiko Matsumiya, Katsunori Hata, Katsuhiko Tsunashima
    • Journal Title

      Journal of Molecular Liquids

      Volume: 203 Pages: 125-130

    • DOI

      10.1016/j.molliq.2014.12.045

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Solvation and electrochemical analyses of neodymium complexes in TFSA-based ionic liquids dissolving the nitrates synthesized from spent Nd-Fe-B magnets2015

    • Author(s)
      Naoko Sasaya, Masahiko Matsumiya, Katsuhiko Tsunashima
    • Journal Title

      Polyhedron

      Volume: 85 Pages: 888-893

    • DOI

      10.1016/j.poly.2014.10.019

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] 湿式分離とイオン液体電析の連携による実廃棄物VCMからの希土類回収技術の開発2014

    • Author(s)
      松宮正彦
    • Journal Title

      溶融塩および高温化学

      Volume: 57(3) Pages: 105-113

    • NAID

      40020289696

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Influence of introducing a benzyl group on physical and electrochemical properties of bis(fluorosulfonyl)amide-based phosphonium ionic liquids2014

    • Author(s)
      Katsuhiko Tsunashima, Chihiro Nagai, Masahiko Matsumiya
    • Journal Title

      ECS Transactions

      Volume: 58(46) Pages: 91-97

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Electrochemical analyses of diffusion behaviors and nucleation mechanisms for neodymium complexes in [DEME][TFSA] ionic liquid2014

    • Author(s)
      Masahiko Matsumiya, Mai Ishii, Ryo Kazama, Satoshi Kawakami
    • Journal Title

      Electrochimica Acta

      Volume: 146 Pages: 371-377

    • DOI

      10.1016/j.electacta.2014.09.066

    • Related Report
      2014 Annual Research Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Recovery of rare earth metals from voice coil motors using bis(trifluoromethylsulfonyl)amide melts by wet separation and electrodeposition2014

    • Author(s)
      Masahiko Matsumiya, Kota Ishioka, Takahiro Yamada, Mai Ishii, Satoshi Kawakami
    • Journal Title

      International Journal of Mineral Processing

      Volume: 126 Pages: 62-69

    • DOI

      10.1016/j.minpro.2013.11.010

    • Related Report
      2014 Annual Research Report 2013 Annual Research Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Development of energy-saving recycling process for rare earth metals from voice coil motor by wet separation and electrodeposition using metallic-TFSA melts2014

    • Author(s)
      Kota Ishioka, Masahiko Matsumiya, Takahiro Yamada, Mai Ishii, Satoshi Kawakami
    • Journal Title

      Hydrometallurgy

      Volume: 144-145 Pages: 186-194

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 湿式分離とイオン液体電析の連携による希土類磁石からのNd, Dyの回収2014

    • Author(s)
      松宮正彦、川上智
    • Journal Title

      セラミックス

      Volume: 49(1) Pages: 22-29

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Physical and electrochemical properties of phosphonium ionic liquids derived from trimethylphosphine2014

    • Author(s)
      Katsuhiko Tsunashima, Yuki Sakai, Masahiko Matsumiya
    • Journal Title

      Electrochemistry Communications

      Volume: 39 Pages: 30-33

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical analysis of diffusion behavior and nucleation mechanism for Dy(II) and Dy(III) in phosphonium-based ionic liquids2013

    • Author(s)
      Ryo Kazama, Masahiko Matsumiya, Nanae Tsuda, Katsuhiko Tsunashima
    • Journal Title

      Electrochimica Acta

      Volume: 113 Pages: 269-279

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Solvation structure of iron group metal ion in TFSA-based ionic liquids investigated by Raman spectroscopy and DFT calculations2013

    • Author(s)
      Masahiko Matsumiya, Yoichi Kamo, Katsunori Hata, Katsuhiko Tsunashima
    • Journal Title

      Journal of Molecular Structure

      Volume: 1048 Pages: 59-63

    • Related Report
      2013 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Attempts to the electrodeposition of Nd from ionic liquids at elevated temperatures2012

    • Author(s)
      近藤瞳、松宮正彦、綱島克彦、小玉春
    • Journal Title

      Electrochimica Acta

      Volume: 66(1) Pages: 313-319

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical behavior and electrodeposition of dysprosium in ionicliquids based on phosphonium cations2012

    • Author(s)
      倉知明史、松宮正彦、綱島克彦、小玉春
    • Journal Title

      Journal of Applied Electrochemistry

      Volume: 42(11) Pages: 961-968

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Investigation of oxidation state of the electrodeposited neodymium metal related with the water content of phosphonium ionic liquids2012

    • Author(s)
      近藤瞳、松宮正彦、綱島克彦、小玉春
    • Journal Title

      ECS Transactions

      Volume: 50(11) Pages: 529-538

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical behavior and solvation analysis of rare earth complexes in ionic liquids media investigated by SECM and Raman spectroscopy2012

    • Author(s)
      津田七瑛、松宮正彦、綱島克彦、小玉春
    • Journal Title

      ECS Transactions

      Volume: 50(11) Pages: 539-548

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Development of recycling process for rare earth magnets by electrodeposition using ionic liquids media2012

    • Author(s)
      石井麻衣、松宮正彦、川上智
    • Journal Title

      ECS Transactions

      Volume: 50(11) Pages: 549-560

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Physicochemical properties of trialkylphosphonium-based protic ionic liquids2012

    • Author(s)
      綱島克彦、福島正弘、松宮正彦
    • Journal Title

      Electrochemistry

      Volume: 80(11) Pages: 904-906

    • NAID

      10031080496

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Presentation] 加温EQCM法の適用性評価及びイオン液体系でのNd(III)還元挙動解明2015

    • Author(s)
      笹屋なお子、松宮正彦、綱島克彦
    • Organizer
      電気化学会第82回大会
    • Place of Presentation
      横浜国立大学
    • Year and Date
      2015-03-15 – 2015-03-17
    • Related Report
      2014 Annual Research Report
  • [Presentation] 沈殿分離/溶媒抽出とイオン液体電析の連携による希土類回収の検討2015

    • Author(s)
      松宮正彦
    • Organizer
      電解科学技術委員会・第95回委員会
    • Place of Presentation
      電気化学会会議室
    • Year and Date
      2015-02-04
    • Related Report
      2014 Annual Research Report
    • Invited
  • [Presentation] ラマン分光法によるアミド系イオン液体中の希土類錯体の配位挙動及び熱力学的解析2014

    • Author(s)
      風間諒、松宮正彦、綱島克彦
    • Organizer
      第46回溶融塩化学討論会
    • Place of Presentation
      かずさアカデミアホール
    • Year and Date
      2014-11-13 – 2014-11-14
    • Related Report
      2014 Annual Research Report
  • [Presentation] 加温EQCM法によるイオン液体系でのNd(III)の還元・析出挙動解析2014

    • Author(s)
      笹屋なお子、松宮正彦、川上智
    • Organizer
      第5回イオン液体討論会
    • Place of Presentation
      横浜シンポジア
    • Year and Date
      2014-10-28 – 2014-10-29
    • Related Report
      2014 Annual Research Report
  • [Presentation] 希土類アミド塩の高純度化とイオン液体電析によるNd-Fe-B磁石からの希土類回収技術の開発2014

    • Author(s)
      米元謙太朗、石岡航太、松宮正彦、川上智
    • Organizer
      第5回イオン液体討論会
    • Place of Presentation
      横浜シンポジア
    • Year and Date
      2014-10-28 – 2014-10-29
    • Related Report
      2014 Annual Research Report
  • [Presentation] 湿式分離とイオン液体電析の連携による実廃棄物VCMからの希土類金属回収技術の開発2014

    • Author(s)
      松宮正彦
    • Organizer
      第185回溶融塩委員会
    • Place of Presentation
      同志社大学
    • Year and Date
      2014-10-23
    • Related Report
      2014 Annual Research Report
    • Invited
  • [Presentation] 湿式分離とイオン液体電析の連携によるNd-Fe-B磁石からの希土類金属の回収2014

    • Author(s)
      松宮正彦、川上智
    • Organizer
      平成26年度資源・素材関係学協会合同秋季大会
    • Place of Presentation
      熊本大学
    • Year and Date
      2014-09-15 – 2014-09-17
    • Related Report
      2014 Annual Research Report
    • Invited
  • [Presentation] 湿式分離とイオン液体電析を融合した省エネルギー型レアアース回収技術の開発2013

    • Author(s)
      松宮正彦、石井麻衣、石岡航太、川上智
    • Organizer
      電気化学会第80回大会
    • Place of Presentation
      東北大学
    • Year and Date
      2013-03-30
    • Related Report
      2012 Annual Research Report
  • [Presentation] 粗視化モデルを導入したイオン液体の分子動力学解析2012

    • Author(s)
      畑克典、鴨陽一、松宮正彦、綱島克彦
    • Organizer
      第35回溶液化学シンポジウム
    • Place of Presentation
      早稲田大学
    • Year and Date
      2012-11-13
    • Related Report
      2012 Annual Research Report
  • [Presentation] Investigation of oxidation state of the electrodeposited neodymium metal relatedwith the water content of phosphonium ionic liquids2012

    • Author(s)
      近藤瞳、松宮正彦、綱島克彦、小玉春
    • Organizer
      222nd Meeting of The Electrochemical Society
    • Place of Presentation
      Hilton Hawaiian Village(Hawaii), USA
    • Year and Date
      2012-10-10
    • Related Report
      2012 Annual Research Report
  • [Presentation] Electrodeposition behavior of rare earth complexes in ionic liquids media investigated by SECM and Raman spectroscopy2012

    • Author(s)
      津田七瑛、松宮正彦、綱島克彦、小玉春
    • Organizer
      222nd Meeting of The Electrochemical Society
    • Place of Presentation
      Hilton Hawaiian Village(Hawaii), USA
    • Year and Date
      2012-10-10
    • Related Report
      2012 Annual Research Report
  • [Presentation] Development of recycling process for rare earth magnets by electrodeposition using ionic liquids media2012

    • Author(s)
      石井麻衣、松宮正彦、川上智
    • Organizer
      222nd Meeting of The Electrochemical Society
    • Place of Presentation
      Hilton Hawaiian village(Hawaii), USA
    • Year and Date
      2012-10-10
    • Related Report
      2012 Annual Research Report
  • [Presentation] イオン液体電析法による廃磁石からの希生類リサイクル技術の開発2012

    • Author(s)
      松宮正彦、石井麻衣、倉知明史、川上智
    • Organizer
      第29回希土類討論会
    • Place of Presentation
      北海道大学
    • Year and Date
      2012-05-15
    • Related Report
      2012 Annual Research Report
  • [Presentation] 実廃棄物voice coil motorからの低温溶融物を利用した省エネルギー型レアアース回収技術の開発2012

    • Author(s)
      石岡航太、松宮正彦、川上智
    • Organizer
      電気化学会第80回大会
    • Place of Presentation
      東北大学
    • Year and Date
      2012-03-29
    • Related Report
      2012 Annual Research Report
  • [Presentation] イオン液体系におけるDy(ll).Dy(III)の拡散挙動及び核生成機構解析2012

    • Author(s)
      風間諒、松宮正彦、綱島克彦
    • Organizer
      電気化学会第80回大会
    • Place of Presentation
      東北大学
    • Year and Date
      2012-03-29
    • Related Report
      2012 Annual Research Report
  • [Presentation] 実廃棄物VCMを利用した希土類TFSA塩回収工程のスケールアップ技術に関する研究

    • Author(s)
      松宮正彦、石岡航太、山田孝大、石井麻衣、川上智
    • Organizer
      電気化学会第81回大会
    • Place of Presentation
      関西大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] 湿式沈殿分離と希土類融解物電析の連携によるNd-Fe-B磁石からの希土類回収技術の開発

    • Author(s)
      石岡航太、石井麻衣、松宮正彦、川上智
    • Organizer
      第45回溶融塩化学討論会
    • Place of Presentation
      慶應義塾大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] イオン液体系におけるNd(III)の電気化学的挙動及び析出機構解析

    • Author(s)
      石井麻衣、石岡航太、松宮正彦、川上智
    • Organizer
      第45回溶融塩化学討論会
    • Place of Presentation
      慶應義塾大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] 走査型電気化学顕微鏡を利用したイオン液体中の遷移金属錯体の電析機構評価

    • Author(s)
      津田七瑛、松宮正彦、綱島克彦
    • Organizer
      第45回溶融塩化学討論会
    • Place of Presentation
      慶應義塾大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] ラマン分光法/定電位電解法の併用によるイオン液体系でのDy(II)/Dy(III)の還元挙動及び配位状態解析

    • Author(s)
      風間諒、津田七瑛、松宮正彦、綱島克彦
    • Organizer
      第45回溶融塩化学討論会
    • Place of Presentation
      慶應義塾大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] 希土類硝酸塩を利用したイオン液体系でのNd(III)の分光及び電気化学的挙動

    • Author(s)
      笹屋なお子、松宮正彦、綱島克彦
    • Organizer
      第4回イオン液体討論会
    • Place of Presentation
      慶應義塾大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] イオン液体系における希土類金属塩の溶解挙動及び熱力学的解析

    • Author(s)
      風間諒、笹屋なお子、松宮正彦、綱島克彦
    • Organizer
      第4回イオン液体討論会
    • Place of Presentation
      慶應義塾大学
    • Related Report
      2013 Annual Research Report
  • [Presentation] 湿式分離とイオン液体電析の連携によるVCMからの希土類リサイクル技術の開発

    • Author(s)
      松宮正彦、石井麻衣、風間諒、川上智
    • Organizer
      第30回希土類討論会
    • Place of Presentation
      北九州国際会議場
    • Related Report
      2013 Annual Research Report
  • [Remarks] 横浜国立大学大学院環境情報研究院松宮研究室

    • URL

      http://www.matsumiya-lab.ynu.ac.jp/

    • Related Report
      2014 Annual Research Report
  • [Remarks] 研究者詳細

    • URL

      http://er-web.jmk.ynu.ac.jp/html/MATSUMIYA_Masahiko/ja.html

    • Related Report
      2014 Annual Research Report
  • [Remarks]

    • URL

      http://www.matumiya-lab.ynu.ac.jp/paperl.html

    • Related Report
      2012 Annual Research Report
  • [Patent(Industrial Property Rights)] イオン液体を利用した希土類元素の回収方法及び希土類元素の回収装置2014

    • Inventor(s)
      松宮正彦、川上智
    • Industrial Property Rights Holder
      国立大学法人横浜国立大学、DOWAホールディングス株式会社
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2014-152291
    • Filing Date
      2014-07-25
    • Related Report
      2014 Annual Research Report
  • [Patent(Industrial Property Rights)] 希土類元素の回収方法及び希土類元素の回収装置2013

    • Inventor(s)
      松宮正彦、川上智
    • Industrial Property Rights Holder
      国立大学法人横浜国立大学、DOWAホールディングス株式会社
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2013-214762
    • Filing Date
      2013-10-15
    • Related Report
      2013 Annual Research Report
  • [Patent(Industrial Property Rights)] 希土類元素の回収方法及び希七類元素の回収装置2012

    • Inventor(s)
      松宮正彦、川上智
    • Industrial Property Rights Holder
      横浜国立大学、DOWAホールディングス株式会社
    • Industrial Property Number
      2012-234202
    • Filing Date
      2012-10-23
    • Related Report
      2012 Annual Research Report

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Published: 2012-04-24   Modified: 2019-07-29  

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