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In-depth understanding of the silicon lithiation process for next-generation lithium secondary batteries

Research Project

Project/Area Number 19K05649
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 36010:Inorganic compounds and inorganic materials chemistry-related
Research InstitutionTottori University

Principal Investigator

Domi Yasuhiro  鳥取大学, 工学研究科, 准教授 (50576717)

Project Period (FY) 2019-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2021: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2020: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2019: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Keywordsリチウム二次電池 / 負極 / ケイ素 / リンドープ / シリサイド / コンポジット化 / イオン液体 / ケイ素系電極 / 金属ケイ化物 / コンポジット / 体積膨張 / ケイ素系負極 / 不純物元素ドープ / 電極/電解質界面 / 軟X線発光分光法 / イオン液体電解液 / 電極-電解質界面 / 反応挙動解析 / ガス・デポジション法
Outline of Research at the Start

Siは次世代のリチウム二次電池用高容量負極としては極めて魅力的であるが,充放電反応にともなう大きな体積変化に起因して乏しいサイクル寿命しか示さない.これまでにある種のイオン液体電解液中におけるSiの過度な体積膨張の抑制,およびSiへの不純物元素のドーピングによるSi内のLi+拡散係数の向上がサイクル性能の改善に寄与することを見出してきたが,その詳細は未だ十分に解明されていない.当該研究では顕微鏡,分光法,および計算化学など種々の解析に基づき上記のサイクル性能向上のメカニズムを明らかにする.また,解析結果に基づき新たなSi系材料の開発指針を示すとともに自ら材料合成にも取組む.

Outline of Final Research Achievements

We thoroughly investigated the mechanism of performance improvement or degradation of Si-based negative electrodes by various analytical methods. In the P-doped Si electrode, which showed good performance, the Li concentration distribution in the Si layer was homogeneous, whereas the Li-Si alloy phase with a large expansion rate was heterogeneously distributed in the Si-alone electrode that deteriorated early. Heterogeneous distribution of the phase caused a local accumulation of high strain and a drastic increment in the thickness of the Si layer, which led to capacity decay. The above results were obtained based on a Si-specific analysis method originally developed in this study. Additionally, the reaction behavior of the silicide electrode and silicide/Si composite electrode was clarified, and based on the obtained knowledge, materials were successfully fabricated to obtain good performance.

Academic Significance and Societal Importance of the Research Achievements

本研究ではリチウム二次電池用Si系負極の反応挙動を徹底解明した.得られた成果に基づき新たな材料設計指針も得られており,一部については実証した.これまで推測の域を超えなかったことを実験事実に基づいて立証した点は学術的に大変意義深い.本研究成果は高エネルギー密度,長寿命,高い安全性および高速充放電性能を兼ね備えた高性能リチウム二次電池を構築するうえで大変重要であり,脱炭素社会の実現に向けて大きく貢献する.

Report

(4 results)
  • 2021 Annual Research Report   Final Research Report ( PDF )
  • 2020 Research-status Report
  • 2019 Research-status Report
  • Research Products

    (32 results)

All 2022 2021 2020 2019 2017 Other

All Journal Article (10 results) (of which Peer Reviewed: 10 results,  Open Access: 6 results) Presentation (17 results) (of which Int'l Joint Research: 1 results,  Invited: 3 results) Book (3 results) Remarks (2 results)

  • [Journal Article] Lithiation and Delithiation Properties of Si-based Electrodes Pre-coated with a Surface Film Derived from an Ionic-liquid Electrolyte2021

    • Author(s)
      Domi Yasuhiro、Usui Hiroyuki、Shindo Yoshiko、Ando Akihiro、Sakaguchi Hiroki
    • Journal Title

      Chemistry Letters

      Volume: 50 Issue: 5 Pages: 1041-1044

    • DOI

      10.1246/cl.210024

    • NAID

      130008040364

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Metallographic Structure Changes in Lanthanum Silicide/Silicon Nanocomposite Electrodes during Lithiation and Delithiation: Implications for Battery Applications2021

    • Author(s)
      Domi Yasuhiro、Usui Hiroyuki、Nishikawa Kei、Sakaguchi Hiroki
    • Journal Title

      ACS Applied Nano Materials

      Volume: 4 Issue: 8 Pages: 8473-8481

    • DOI

      10.1021/acsanm.1c01765

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Lithiation/Delithiation Properties of Lithium Silicide Electrodes in Ionic-Liquid Electrolytes2021

    • Author(s)
      Domi Yasuhiro、Usui Hiroyuki、Ieuji Naoya、Nishikawa Kei、Sakaguchi Hiroki
    • Journal Title

      ACS Applied Materials & Interfaces

      Volume: 13 Issue: 3 Pages: 3816-3824

    • DOI

      10.1021/acsami.0c17552

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Electrochemical Lithiation and Delithiation Properties of FeSi<sub>2</sub>/Si Composite Electrodes in Ionic-Liquid Electrolytes2020

    • Author(s)
      DOMI Yasuhiro、USUI Hiroyuki、SHINDO Yoshiko、YODOYA Shuhei、SATO Hironori、NISHIKAWA Kei、SAKAGUCHI Hiroki
    • Journal Title

      Electrochemistry

      Volume: 88 Issue: 6 Pages: 548-554

    • DOI

      10.5796/electrochemistry.20-00091

    • NAID

      130007936844

    • ISSN
      1344-3542, 2186-2451
    • Year and Date
      2020-11-05
    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effect of Element Substitution on Electrochemical Performance of Silicide/Si Composite Electrodes for Lithium-Ion Batteries2020

    • Author(s)
      Domi Yasuhiro、Usui Hiroyuki、Nakabayashi Eisuke、Kimura Yuta、Sakaguchi Hiroki
    • Journal Title

      ACS Applied Energy Materials

      Volume: 3 Issue: 8 Pages: 7438-7444

    • DOI

      10.1021/acsaem.0c00846

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Reaction Behavior of a Silicide Electrode with Lithium in an Ionic-Liquid Electrolyte2020

    • Author(s)
      Domi Yasuhiro、Usui Hiroyuki、Sugimoto Kai、Gotoh Kazuma、Nishikawa Kei、Sakaguchi Hiroki
    • Journal Title

      ACS Omega

      Volume: 5 Issue: 35 Pages: 22631-22636

    • DOI

      10.1021/acsomega.0c03357

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Analysis of the Li Distribution in Si-Based Negative Electrodes for Lithium-Ion Batteries by Soft X-ray Emission Spectroscopy2020

    • Author(s)
      Domi Yasuhiro、Usui Hiroyuki、Ando Akihiro、Nishikawa Kei、Sakaguchi Hiroki
    • Journal Title

      ACS Applied Energy Materials

      Volume: 3 Issue: 9 Pages: 8619-8626

    • DOI

      10.1021/acsaem.0c01238

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Piperidinium-Based Ionic Liquids as an Electrolyte Solvent for Li-Ion Batteries: Effect of Number and Position of Oxygen Atom in Cation Side Chain on Electrolyte Property2020

    • Author(s)
      Shimizu Masahiro、Yamaguchi Kazuki、Usui Hiroyuki、Ieuji Naoya、Yamashita Takuya、Komura Takuro、Domi Yasuhiro、Nokami Toshiki、Itoh Toshiyuki、Sakaguchi Hiroki
    • Journal Title

      Journal of The Electrochemical Society

      Volume: 167 Issue: 7 Pages: 070516-070516

    • DOI

      10.1149/1945-7111/ab6a89

    • NAID

      120007184157

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Potassiation and Depotassioation Properties of Sn<sub>4</sub>P<sub>3</sub> Electrode in an Ionic-Liquid Electrolyte2019

    • Author(s)
      DOMI Yasuhiro、USUI Hiroyuki、NAKABAYASHI Eisuke、YAMAMOTO Takayuki、NOHIRA Toshiyuki、SAKAGUCHI Hiroki
    • Journal Title

      Electrochemistry

      Volume: 87 Issue: 6 Pages: 333-335

    • DOI

      10.5796/electrochemistry.19-00052

    • NAID

      130007741815

    • ISSN
      1344-3542, 2186-2451
    • Year and Date
      2019-11-05
    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effect of Mechanical Pre-Lithiation on Electrochemical Performance of Silicon Negative Electrode for Lithium-Ion Batteries2017

    • Author(s)
      Yasuhiro Domi, Hiroyuki Usui, Daichi Iwanari, Hiroki Sakaguchi
    • Journal Title

      Journal of The Electrochemical Society

      Volume: 164 Issue: 7 Pages: 040512-040512

    • DOI

      10.1149/2.1361707jes

    • NAID

      120006523089

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] ケイ素と機能の異なる二種類のシリサイドからなる電極のリチウム二次電池負極特性2022

    • Author(s)
      〇道見康弘,薄井洋行,岡阪拓親,西川慶,坂口裕樹
    • Organizer
      2022年電気化学会第89回大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] リチウム二次電池用遷移金属ケイ化物電極のLi吸蔵-放出機構の解明2021

    • Author(s)
      〇安藤匠海,道見康弘,薄井洋行,後藤和馬,坂口裕樹
    • Organizer
      第10回JACI/GSCシンポジウム
    • Related Report
      2021 Annual Research Report
  • [Presentation] 機能の異なる二種のシリサイドを含有するケイ素系電極のリチウム二次電池負極特性2021

    • Author(s)
      〇岡阪拓親,道見康弘,薄井洋行,西川慶,坂口裕樹
    • Organizer
      2021年電気化学秋季大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] リチウム二次電池負極用Si粒子における膨張の異方性とその抑制2021

    • Author(s)
      〇中野拓磨,道見康弘,薄井洋行,安藤明寛,西川慶,坂口裕樹
    • Organizer
      第62回電池討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] リチウム二次電池用遷移金属ケイ化物電極の充放電メカニズムの解明2021

    • Author(s)
      〇安藤匠海,道見康弘,薄井洋行,後藤和馬,西川慶,坂口裕樹
    • Organizer
      第62回電池討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] ケイ素系負極活物質の創製とSiに特化した分析法2021

    • Author(s)
      〇道見康弘,坂口裕樹
    • Organizer
      第409回電池技術委員会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] 機能の異なる二種のシリサイドを含有するSi系電極のリチウム二次電池負極特性2021

    • Author(s)
      〇岡阪拓親,道見康弘,薄井洋行,西川慶,坂口裕樹
    • Organizer
      令和3年度 第3回関西電気化学研究会
    • Related Report
      2021 Annual Research Report
  • [Presentation] リチウム二次電池用Si系負極の反応メカニズムの解明2021

    • Author(s)
      道見康弘,薄井洋行,坂口裕樹
    • Organizer
      第4回 岡山大学 次世代電池材料研究会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Presentation] リチウムケイ化物からなる負極の電気化学的性質2021

    • Author(s)
      道見康弘,薄井洋行,家氏直哉,西川慶,坂口裕樹
    • Organizer
      2021年電気化学会第88回大会
    • Related Report
      2020 Research-status Report
  • [Presentation] リチウム二次電池用希土類シリサイド-ケイ素コンポジット電極の反応挙動解析2020

    • Author(s)
      道見康弘,薄井洋行,中林永丞, 坂口裕樹
    • Organizer
      第36回希土類討論会
    • Related Report
      2020 Research-status Report
  • [Presentation] リチウム二次電池用遷移金属ケイ化物電極の電気化学的Li吸蔵-放出メカニズムの解明2020

    • Author(s)
      道見康弘,薄井洋行,杉本海,後藤和馬,西川慶,坂口裕樹
    • Organizer
      第61回電池討論会
    • Related Report
      2020 Research-status Report
  • [Presentation] リチウム二次電池用ケイ化物電極のLi吸蔵-放出機構の解明2020

    • Author(s)
      道見康弘,薄井洋行,杉本海,後藤和馬, 坂口裕樹
    • Organizer
      2020年電気化学会第87回大会
    • Related Report
      2019 Research-status Report
  • [Presentation] 次世代リチウム二次電池のためのケイ素系負極活物質の創製と電極-電解質界面の最適化2019

    • Author(s)
      道見 康弘
    • Organizer
      平成30年度日本材料学会中国支部 支部学術奨励賞 受賞講演
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] イオン液体電解液中における希土類シリサイド電極のリチウム二次電池負極特性2019

    • Author(s)
      道見康弘,薄井洋行,高石玲奈,坂口裕樹
    • Organizer
      第35回希土類討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] Significant Suppression of Silicon Negative Electrode for Lithium-Ion Battery in Ionic-Liquid Electrolyte2019

    • Author(s)
      Yasuhiro Domi, Hiroyuki Usui, Kazuki Yamaguchi, Shuhei Yodoya, and Hiroki Sakaguchi
    • Organizer
      The Electrochemical Conference on Energy and the Environment: Bioelectrochemistry and Energy Storage (ECEE 2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] 電解液の違いがリチウム二次電池用Si負極の体積膨張におよぼす影響2019

    • Author(s)
      道見康弘,薄井洋行,山口和輝,淀谷周平,安藤明寛,坂口裕樹
    • Organizer
      2019年電気化学秋季大会
    • Related Report
      2019 Research-status Report
  • [Presentation] リチウム二次電池用Si系負極の体積膨張メカニズム解明とその抑制2019

    • Author(s)
      道見 康弘,薄井 洋行,山口和輝、淀谷周平、 安藤明寛、坂口 裕樹
    • Organizer
      第60回電池討論会
    • Related Report
      2019 Research-status Report
  • [Book] モビリティ用電池の化学2022

    • Author(s)
      道見康弘、薄井洋行、坂口裕樹
    • Total Pages
      200
    • Publisher
      化学同人
    • ISBN
      9784759814040
    • Related Report
      2021 Annual Research Report
  • [Book] 全固体電池の界面抵抗低減と作製プロセス、評価技術2020

    • Author(s)
      道見康弘,薄井洋行,坂口裕樹
    • Total Pages
      490
    • Publisher
      技術情報協会
    • ISBN
      9784861047800
    • Related Report
      2019 Research-status Report
  • [Book] リチウムイオン二次電池用シリコン系負極材の開発動向2019

    • Author(s)
      道見康弘,薄井洋行,坂口裕樹
    • Total Pages
      251
    • Publisher
      シーエムシー出版
    • ISBN
      9784781314853
    • Related Report
      2019 Research-status Report
  • [Remarks] 坂口研究室

    • URL

      http://www.chem.tottori-u.ac.jp/~sakaguchi/index.html

    • Related Report
      2021 Annual Research Report
  • [Remarks] 坂口研究室 学会・出版リスト

    • URL

      http://www.chem.tottori-u.ac.jp/~sakaguchi/research_j.html

    • Related Report
      2020 Research-status Report 2019 Research-status Report

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Published: 2019-04-18   Modified: 2023-01-30  

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