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Development of Ti-S-based n-type thermoelectric materials

Research Project

Project/Area Number 17H04951
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypeSingle-year Grants
Research Field Inorganic materials/Physical properties
Research InstitutionKyushu University

Principal Investigator

Koichiro Suekuni  九州大学, 総合理工学研究院, 准教授 (10582926)

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥24,050,000 (Direct Cost: ¥18,500,000、Indirect Cost: ¥5,550,000)
Fiscal Year 2019: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2018: ¥7,670,000 (Direct Cost: ¥5,900,000、Indirect Cost: ¥1,770,000)
Fiscal Year 2017: ¥14,560,000 (Direct Cost: ¥11,200,000、Indirect Cost: ¥3,360,000)
Keywords熱電材料 / 熱電物性 / チタン硫化物 / ゼーベック係数 / 出力因子 / 電子構造 / 半導体 / 熱電変換 / 硫化物 / スピネル / 層状物質
Outline of Final Research Achievements

In this study, we aimed to develop novel n-type thermoelectric (TE) materials and to propose design guidelines for TE materials with excellent electronic properties. For the purpose, the TE properties and electronic structures were investigated for the materials with structural networks composed of edge-sharing TiS6 octahedra, namely Cu2Ti4S8 spinel and its related materials, layered materials (SnS)1.2(TiS2)n (n=1,2), and a quasi-one-dimensional material Sn1.2Ti0.8S3. N-type electronic properties arising from TiS6 network were observed for all the materials, for which the electron carrier concentration was tuned by elemental substitutions and oxidative extraction of Cu. As a result, TE figures of merit for the materials were enhanced. These results demonstrate that materials with TiS6 octahedral networks are promising as n-type TE materials. Furthermore, it was found that the substitution of Co for Ti in Cu2Ti4S8 was effective for improving electronic properties.

Academic Significance and Societal Importance of the Research Achievements

熱電材料は未利用熱からの電力回収(熱電発電)への応用が期待されている。本研究では,チタンー硫黄系物質に着目し,その熱電物性を系統的に調べた。その結果,TiS6八面体の稜共有ネットワークを有する物質では,伝導帯を構成する電子軌道が類似すること,その電子構造がn型の電気的特性の発現に有利であることが判った。また,原子サイトへの空孔導入や元素置換などの方法により電子キャリア濃度を制御でき,熱電性能を高められることを確認した。得られた知見は,さらに高性能な熱電材料の開発に結び付くものと期待される。

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (35 results)

All 2020 2019 2018 2017

All Journal Article (7 results) (of which Peer Reviewed: 6 results) Presentation (28 results) (of which Int'l Joint Research: 8 results,  Invited: 7 results)

  • [Journal Article] A strategy for boosting the thermoelectric performance of famatinite Cu3SbS42020

    • Author(s)
      Taiki Tanishita, Koichiro Suekuni, Hirotaka Nishiate, Chul-Ho Lee, Michitaka Ohtaki
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Issue: 4 Pages: 2081-2086

    • DOI

      10.1039/c9cp06233e

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Enargite Cu3PS4: A Cu-S-Based Thermoelectric Material with a Wurtzite-Derivative Structure2020

    • Author(s)
      Takuya Tanimoto, Koichiro Suekuni, Taiki Tanishita, Hidetomo Usui, Terumasa Tadano, Taiga Kamei, Hikaru Saito, Hirotaka Nishiate, Chul-Ho Lee, Kazuhiko Kuroki, Michitaka Ohtaki
    • Journal Title

      Advanced Functional Materials

      Volume: - Issue: 22

    • DOI

      10.1002/adfm.202000973

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electronic structure and thermoelectric properties of Sn1.2-xNbxTi0.8S3 with a quasi-one-dimensional structure2019

    • Author(s)
      Koichiro Suekuni, Hidetomo Usui, Siying Qiao, Katsuaki Hashikuni, Tatsuya Hirano, Hirotaka Nishiate, Chul-Ho Lee, Kazuhiko Kuroki, Kosuke Watanabe, Michitaka Ohtaki
    • Journal Title

      Journal of Applied Physics

      Volume: 125 Issue: 17 Pages: 175111-175111

    • DOI

      10.1063/1.5093183

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Thermoelectric Properties and Electronic Structures of CuTi2S4 Thiospinel and Its Derivatives: Structural Design for Spinel-Related Thermoelectric Materials2019

    • Author(s)
      Katsuaki Hashikuni, Koichiro Suekuni, Hidetomo Usui, Raju Chetty, Michihiro Ohta, Kazuhiko Kuroki, Toshiro Takabatake, Kosuke Watanabe, and Michitaka Ohtaki
    • Journal Title

      Inorganic Chemistry

      Volume: 58 Issue: 2 Pages: 1425-1432

    • DOI

      10.1021/acs.inorgchem.8b02955

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Atomic-scale phonon scatterers in thermoelectric colusites with a tetrahedral framework structure2019

    • Author(s)
      Suekuni Koichiro、Shimizu Yuta、Nishibori Eiji、Kasai Hidetaka、Saito Hikaru、Yoshimoto Daichi、Hashikuni Katsuaki、Bouyrie Yohan、Chetty Raju、Ohta Michihiro、Guilmeau Emmanuel、Takabatake Toshiro、Watanabe Kosuke、Ohtaki Michitaka
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 7 Issue: 1 Pages: 228-235

    • DOI

      10.1039/c8ta08248k

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Carrier concentration tuning in thermoelectric thiospinel Cu2CoTi3S8 by oxidative extraction of copper2018

    • Author(s)
      Katsuaki Hashikuni, Koichiro Suekuni, Kosuke Watanabe, Yohan Bouyrie, Michihiro Ohta, Michitaka Ohtaki, Toshiro Takabatake
    • Journal Title

      Journal of Solid State Chemistry

      Volume: 259 Pages: 5-10

    • DOI

      10.1016/j.jssc.2017.12.031

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 天然硫化銅鉱物を模した熱電物質の開発2017

    • Author(s)
      末國晃一郎
    • Journal Title

      日本熱電学会誌

      Volume: 13 Pages: 149-154

    • Related Report
      2017 Annual Research Report
  • [Presentation] 硫化スピネルCu2FeTi3S8の結晶構造と熱電物性に対するCu欠損効果2019

    • Author(s)
      橋國克明, 末國晃一郎, ChettyRaju, 太田道広, 高畠敏郎, 大瀧倫卓
    • Organizer
      第16回日本熱電学会学術講演会(TSJ2019)
    • Related Report
      2019 Annual Research Report
  • [Presentation] ファマチナイトCu3Sb1-x-yGexPyS4の高い熱電性能2019

    • Author(s)
      谷下太基, 末國晃一郎, 西当弘隆, 李哲虎, 大 瀧倫卓
    • Organizer
      第16回日本熱電学会学術講演会(TSJ2019)
    • Related Report
      2019 Annual Research Report
  • [Presentation] エナーガイトCu3PS4におけるPのGe置換によるキャリア濃度制御2019

    • Author(s)
      谷本拓哉, 谷下太基, 末國晃一郎, 臼井秀知, 西当弘隆, 李哲虎, 黒木 和彦, 大瀧倫卓
    • Organizer
      第16回日本熱電学会学術講演会(TSJ2019)
    • Related Report
      2019 Annual Research Report
  • [Presentation] コルーサイトCu26V2Si6S32の合成とキャリア濃度制御2019

    • Author(s)
      清水裕太, 末國晃一郎, ChettyRaju, 太田道広, 高畠敏郎, 大瀧倫卓
    • Organizer
      第16回日本熱電学会学術講演会(TSJ2019)
    • Related Report
      2019 Annual Research Report
  • [Presentation] Rhombohedral CuTi2S4: a thiospinel derived thermoelectric material2019

    • Author(s)
      Katsuaki Hashikuni, Koichiro Suekuni, Hidetomo Usui, Raju Chetty, Michihiro Ohta, Kazuhiko Kuroki, Toshiro Takabatake, Kosuke Watanabe, Michitaka Ohtaki
    • Organizer
      The 38th International Conference and the 4th Asian Conference on Thermoelectrics (ICT/ACT2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Quasi one dimensional electronic structure and low thermal conductivity in Sn1.2Ti0.8S32019

    • Author(s)
      Koichiro Suekuni, Hidetomo Usui, Siying Qiao, Katsuaki Hashikuni, Tatsuya Hirano, Hirotaka Nishiate, Chul-Ho Lee, Kazuhiko Kuroki, Kosuke Watanabe, Michitaka Ohtaki
    • Organizer
      The 38th International Conference and the 4th Asian Conference on Thermoelectrics (ICT/ACT2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] M-site substitution effects on the thermoelectric properties of Cu26Nb2M6S32 (M = Sn, Ge, Si) colusite2019

    • Author(s)
      Yuta Shimizu, Koichiro Suekuni, Raju Chetty, Michihiro Ohta, Toshiro Takabatake, Kosuke Watanabe, Michitaka Ohtaki
    • Organizer
      The 38th International Conference and the 4th Asian Conference on Thermoelectrics (ICT/ACT2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Naturally-occurring minerals for thermoelectric power generation2019

    • Author(s)
      Koichiro Suekuni
    • Organizer
      International workshop Emergent Condensed-Matter Physics 2019 (ECMP2019)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Thermoelectric Properties of Cubic and Rhombohedral CuTi2S42019

    • Author(s)
      K. Hashikuni, K. Suekuni, H. Usui, R. Chetty, M. Ohta, K. Kuroki, T. Takabatake, K. Watanabe, and M. Ohtaki
    • Organizer
      International workshop Emergent Condensed-Matter Physics 2019 (ECMP2019)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Interplay between the structural and thermoelectric properties in Cu-S based synthetic minerals2018

    • Author(s)
      Koichiro Suekuni
    • Organizer
      37th International and 16th European Conference on Thermoelectrics (ICT2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 熱電硫化銅鉱物の開発2018

    • Author(s)
      末國晃一郎
    • Organizer
      第15回日本熱電学会学術講演会(TSJ2018)
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 硫化スピネルCu2Ti4S8の結晶構造と電子構造および熱電物性に対するCu欠損効果2018

    • Author(s)
      橋國克明, 末國晃一郎, 臼井秀知, Chetty Raju, 太田道広, 黒木和彦, 高畠敏郎
    • Organizer
      第15回日本熱電学会学術講演会(TSJ2018)
    • Related Report
      2018 Annual Research Report
  • [Presentation] 擬一次元構造をとるSn1.2Ti0.8S3とSn1.0Zr1.0S3の熱電物性に対するNb 置換効果2018

    • Author(s)
      喬思瑩, 末國晃一郎, 西当弘隆, 李哲虎, 大瀧倫卓
    • Organizer
      第15回日本熱電学会学術講演会(TSJ2018)
    • Related Report
      2018 Annual Research Report
  • [Presentation] 熱電硫化銅鉱物コルーサイトの低熱伝導率を実現する結晶構造2018

    • Author(s)
      清水裕太, 末國晃一郎, 斎藤光, 吉本大地, 西堀英治, 笠井秀隆, Bouyrie Yohan, Chetty Raju, 太田道広, 橋國克明, 高畠敏郎, 大瀧倫卓
    • Organizer
      第15回日本熱電学会学術講演会(TSJ2018)
    • Related Report
      2018 Annual Research Report
  • [Presentation] ミスフィット層状化合物(SnS)1.2(TiS2)n (n = 1, 2)の熱電物性に対する元素置換効果2018

    • Author(s)
      平野達也, 末國晃一郎, 橋國克明, 西当弘隆, 李哲虎, 大瀧倫卓
    • Organizer
      第55回化学関連支部合同九州大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 熱電硫化銅鉱物コルーサイトの結晶構造と熱電特性の制御2018

    • Author(s)
      清水裕太, 末國晃一郎, 斉藤光, 吉本大地, Bouyrie Yohan, 太田道広, 橋國克明, 高畠敏郎, 波多聰, 大瀧倫卓
    • Organizer
      第55回化学関連支部合同九州大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Effects of Se substitution on the thermoelectric properties of (SnS)1.2(TiS2)n (n = 1, 2)2018

    • Author(s)
      Tatsuya Hirano, Koichiro Suekuni, Katsuaki Hashikuni, Hirotaka Nishiate, Chul-Ho Lee, Toshiro Takabatake, Michitaka Ohtaki
    • Organizer
      37th International and 16th European Conference on Thermoelectrics (ICT2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Thermoelectric Properties of Cu-deficient Thiospinel Cu2-xTi4S8 and the derivative Cu2-xTi4.5S82018

    • Author(s)
      Katsuaki Hashikuni, Koichiro Suekuni, Hidetomo Usui, Raju Chetty, Michihiro Ohta, Kazuhiko Kuroki, Toshiro Takabatake
    • Organizer
      37th International and 16th European Conference on Thermoelectrics (ICT2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 高性能熱電物質の探索2018

    • Author(s)
      末國晃一郎
    • Organizer
      日本物理学会 第73回年次大会(2018年)
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Cu-S and Ti-S based thermoelectric materials2017

    • Author(s)
      K. Suekuni, M. Ohta, T. Takabatake, M. Ohtaki
    • Organizer
      International Union of Materials Research Society-International Conference of Advanced Materials (IUMRS-ICAM) 2017
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] 環境調和型熱電硫化物の構造・電子・フォノン物性2017

    • Author(s)
      末國晃一郎
    • Organizer
      第32回九工大物性グループセミナー
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Cu-S 系および Ti-S 系硫化物の構造と熱電物性2017

    • Author(s)
      末國晃一郎
    • Organizer
      日本熱電学会第22回研究会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] 熱電硫化物研究の最前線2017

    • Author(s)
      末國晃一郎
    • Organizer
      秋田熱電材料研究会第2回講演会イン湯沢
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Carrier density tuning in Cu2CoTi3S8 by oxidative extraction of Cu2017

    • Author(s)
      K. Hashikuni, K. Suekuni, K. Watanabe, Y. Bouyrie, M. Ohta, M. Ohtaki, T. Takabatake
    • Organizer
      36th Annual International Conference on Thermoelectrics (ICT2017)
    • Related Report
      2017 Annual Research Report
  • [Presentation] Ti-S 系物質の構造次元性と熱電物性2017

    • Author(s)
      末國晃一郎, 臼井秀知, 関水準記, 橋國克明, 喬 思瑩, 平野達也, 黒木和彦, 高畠敏郎, 大瀧倫卓
    • Organizer
      第14回日本熱電学会学術講演会(TSJ2017)
    • Related Report
      2017 Annual Research Report
  • [Presentation] N型チオスピネルCu2CoTi3S8のCuのヨウ素酸化抽出によるキャリア密度制御2017

    • Author(s)
      橋國克明, 末國晃一郎, 渡邊厚介, Bouyrie, Y., 太田道広, 大瀧倫卓, 高畠敏郎
    • Organizer
      第14回日本熱電学会学術講演会(TSJ2017)
    • Related Report
      2017 Annual Research Report
  • [Presentation] ミスフィット層状化合物(SnS)1.2(TiS2)n (n=1, 2)の熱電物性に対するSe置換効果2017

    • Author(s)
      平野達也, 末國晃一郎, 橋國克明, 高畠敏郎, 西当弘隆, 李 哲虎, 大瀧倫卓
    • Organizer
      第14回日本熱電学会学術講演会(TSJ2017)
    • Related Report
      2017 Annual Research Report
  • [Presentation] 擬一次元物質Sn1.2Ti0.8S3の熱電物性に対するNb置換効果2017

    • Author(s)
      喬思瑩, 末國晃一郎, 平野達也, 橋國克明, 高畠敏郎, 西当弘隆, 李 哲虎, 大瀧倫卓
    • Organizer
      第14回日本熱電学会学術講演会(TSJ2017)
    • Related Report
      2017 Annual Research Report

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Published: 2017-04-28   Modified: 2021-02-19  

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