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Seebeck effect of conducting polymers and development of efficient organic thermoelectric devices

Research Project

Project/Area Number 17K05965
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Energy-related chemistry
Research InstitutionHiroshima University

Principal Investigator

Harima Yutaka  広島大学, 工学研究科, 名誉教授 (20156524)

Co-Investigator(Kenkyū-buntansha) 今榮 一郎  広島大学, 工学研究科, 准教授 (90293399)
Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2019: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2018: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2017: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Keywords熱電変換 / ゼーベック効果 / 導電性高分子 / 有機材料 / ドープ率 / 位置規則性 / EDOT:PSS / ゼーベック係数 / PEDOT:PSS / 有機熱電材料 / 電気伝導度 / 電気化学 / 熱電効果 / Seebeck係数 / 熱電材料
Outline of Final Research Achievements

Relationship between the Seebeck coefficient (S) and charge density (doping level) in conductive polymers was studied in order to create highly efficient organic thermoelectric materials. In regioregular poly(3-hexylthiophene) (P3HT) films, the relationship between log S and the doping level gave a straight line with a slope of -1 over a wide range of doping level. This was the first reliable result of the correlation between the charge density and S among those observed for inorganic and organic thermoelectric materials so far. The finding had a strong impact on researchers in the field of thermoelectricity. We extended the target to regiorandom P3HT synthesized by polycondensation and electro-oxidation polymerization, and the doping level dependence of S was studied. We extended further our research focus to PEDOT:PSS, which is a promising organic thermoelectric conversion material, and investigated the search for efficient organic thermoelectric materials.

Academic Significance and Societal Importance of the Research Achievements

化石燃料に代わる再生可能エネルギーへの関心は強さを増している。太陽光発電や風力発電と並んで排熱の利用技術,特に低温領域での熱電材料の開発が喫緊の課題となっている。本研究課題では有機材料の中でも特に優れた特徴を有する導電性高分子を対象に,熱電変換特性に重要な影響を与えるゼーベック係数(S)に着目した。ドープ率の評価に電気化学的手法を用いることにより,位置規則性を有するP3HT膜ではlog Sとドープ率の間に直線関係が成り立ち,その傾きは-1であることを見出した。金属等に対して理論的に予測される-2/3とわずかに異なる勾配のを解明することは学術的に意義深く,高効率有機熱電変換素子の開発にも資する。

Report

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

    (30 results)

All 2020 2019 2018 2017

All Journal Article (11 results) (of which Peer Reviewed: 11 results) Presentation (16 results) (of which Int'l Joint Research: 7 results) Patent(Industrial Property Rights) (3 results)

  • [Journal Article] Tuning of electronic properties of novel donor-acceptor polymers containing oligothiophenes with electron-withdrawing ester groups2020

    • Author(s)
      I. Imae, N. Tada, Y. Harima
    • Journal Title

      Polymer Bulletin

      Volume: - Issue: 5 Pages: 2341-2355

    • DOI

      10.1007/s00289-020-03212-5

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Thermoelectric properties of poly(3,4-ethylenedioxythiophene) with fluorine-containing polyanion as a dopant2020

    • Author(s)
      I. Imae, T. Goto, Y. Ooyama, Y. Harima
    • Journal Title

      Polymer

      Volume: -

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis and Properties of Donor-acceptor-type Polymers Comprising Alkoxy-substituted Bithiophene Units2019

    • Author(s)
      I. Imae, N. Tada, and Y. Harima
    • Journal Title

      Journal of Photopolymer Science and Technology

      Volume: 32 Issue: 4 Pages: 585-592

    • DOI

      10.2494/photopolymer.32.585

    • NAID

      130007744437

    • ISSN
      0914-9244, 1349-6336
    • Year and Date
      2019-06-24
    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Flexible thermoelectric materials based on conducting polymers doped with silicone polymer electrolyte2019

    • Author(s)
      I. Imae, H. Kataoka, Y. Harima
    • Journal Title

      Molecular Crystals and Liquid Crystals

      Volume: 685 Issue: 1 Pages: 100-106

    • DOI

      10.1080/15421406.2019.1645467

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Molecular properties of thiophene-based donor-acceptor-donor small molecules with well-defined structures2019

    • Author(s)
      I. Imae, M. Kumano, Y. Harima
    • Journal Title

      Science of Advanced Materials

      Volume: 11 Issue: 6 Pages: 792-799

    • DOI

      10.1166/sam.2019.3507

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Seebeck coefficients of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) correlated with oxidation levels2019

    • Author(s)
      Ichiro Imae, Mengyan Shi, Yousuke Ooyama, Yutaka Harima
    • Journal Title

      J. Phys. Chem. C

      Volume: 123 Issue: 7 Pages: 4002-4006

    • DOI

      10.1021/acs.jpcc.8b10956

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Thermoelectric properties of polythiophenes partially substituted by ethylenedioxy groups2018

    • Author(s)
      Ichiro Imae, Takashi Koumoto, Yutaka Harima
    • Journal Title

      polymer

      Volume: 144 Pages: 43-50

    • DOI

      10.1016/j.polymer.2018.04.031

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Seebeck coefficients of regioregular poly(3-hexylthiophene) correlated with doping levels2018

    • Author(s)
      Imae Ichiro、Akazawa Ryosuke、Harima Yutaka
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 20 Issue: 2 Pages: 738-741

    • DOI

      10.1039/c7cp07114k

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Fine-tuning of electronic properties in donor?acceptor conjugated polymers based on oligothiophenes2017

    • Author(s)
      Imae Ichiro、Sagawa Hitoshi、Harima Yutaka
    • Journal Title

      Japanese Journal of Applied Physics

      Volume: 57 Issue: 3S2 Pages: 03EJ01-03EJ01

    • DOI

      10.7567/jjap.57.03ej01

    • NAID

      210000148781

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Highly improved thermoelectric performances of PEDOT:PSS/SWCNT composites by solvent treatment2017

    • Author(s)
      Zhang Lu、Harima Yutaka、Imae Ichiro
    • Journal Title

      Organic Electronics

      Volume: 51 Pages: 304-307

    • DOI

      10.1016/j.orgel.2017.09.030

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Electrosynthesis of a multilayer film stacked alternately by poly(3,4-ethylenedioxythiophene) and reduced graphene oxide from aqueous solution2017

    • Author(s)
      Imae Ichiro、Fujimoto Daiki、Zhang Lu、Harima Yutaka
    • Journal Title

      Electrochemistry Communications

      Volume: 81 Pages: 65-69

    • DOI

      10.1016/j.elecom.2017.06.005

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Presentation] Synthesis and properties of donor-acceptor-type polymers having alkoxyl-substituted bithiophenes2019

    • Author(s)
      I. Imae, Naofumi, Tada, Y. Harima
    • Organizer
      36th international conference of photopolymer science and technology (ICPST-36)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Tuning of electronic properties of novel donor-acceptor polymers having oligothiophenes with electron-withdrawing ester groups2019

    • Author(s)
      I. Imae, N. Tada, Y. Harima
    • Organizer
      10th international conference on molecular electronics and bioelectronics (M&BE 10)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Seebeck Coefficients of Conducting Polyn1ers Correlated with Doping Levels2018

    • Author(s)
      Ichiro Imae, Ryosuke Akazawa, Mengyan Shi, Yutaka Harima,
    • Organizer
      2018 International Conference on Thermoelectrics (2018 ICT)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Flexible Thermoelectric Materials Based on Conducting Polyn1ers Doped with Silicone Polymer Electrolyte2018

    • Author(s)
      Ichiro Imae, Hiroki Kataoka, Yutaka Harima
    • Organizer
      2018 KJF International Conference on Organic Materials for Electronics and Photonics
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Thermoelectric Properties of Conducting Polymers with Controlled Doping Levels2018

    • Author(s)
      Ichiro Imae, Ryosuke Akazawa, Mengyan Shi, Yutaka Harima
    • Organizer
      12th SPSJ International Polymer Conference (IPC2018)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] アルキル置換ポリチオフェンの熱電変換特性におけるドープ率依存性2018

    • Author(s)
      今榮一郎、赤津亮介、播磨裕
    • Organizer
      第67回高分子学会年次大会
    • Related Report
      2018 Research-status Report
  • [Presentation] ポリ(3,4-エチレンジオキシチオフヱン):ポリ(スチレンスルホン酸)(PEDOT:PSS)の熱電変換特性に及ぼす酸化率依存性2018

    • Author(s)
      今榮 一郎、石多燕、大山陽介、播磨裕
    • Organizer
      第67回高分子討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] 酸化率を制御したPEDOT:PSSの熱電変換特性2018

    • Author(s)
      今榮 一郎、石多燕、大山陽介、播磨裕
    • Organizer
      第79回応用物理学会秋季学術講演会
    • Related Report
      2018 Research-status Report
  • [Presentation] PEDOT:PSSの熱電変換特性のドープ率依存性2018

    • Author(s)
      今榮一郎、石梦燕、大山陽介、播磨裕
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Research-status Report
  • [Presentation] 電気化学的手法によりドープ率を制御したポリヘキシルチオフェンの熱電変換特性2017

    • Author(s)
      今榮一郎、赤澤亮介、播磨裕
    • Organizer
      第14回日本熱電学会学術講演会
    • Related Report
      2017 Research-status Report
  • [Presentation] ポリ(3-ヘキシルチオフェン)のドープ率評価と熱電変換特性2017

    • Author(s)
      今榮一郎、赤澤亮介、播磨裕
    • Organizer
      第66回高分子討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] 高い熱電変換能を有するPEDOT/SWCNT複合体の簡便合成法の開発2017

    • Author(s)
      今榮一郎、張露、播磨裕
    • Organizer
      第14回日本熱電学会学術講演会
    • Related Report
      2017 Research-status Report
  • [Presentation] PEDOT/グラフェン交互積層膜の簡便な合成法の開発2017

    • Author(s)
      今榮一郎、藤本大樹、播磨裕
    • Organizer
      第66回高分子討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] 簡便な手法により作製した導電性高分子/カーボンナノチューブ複合膜の熱電変換特性2017

    • Author(s)
      今榮一郎、張露、播磨裕
    • Organizer
      第36回無機高分子研究討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Synthesis and Photovoltaic Performances of Novel D-A Copolymers Having Oligothiophenes Partially Containing 3,4-Ethylenedioxythiophene2017

    • Author(s)
      I. Imae, H. Sagawa, Y. Harima
    • Organizer
      9th International Conference on Molecular Electronics and Bioelectronics
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Tuning of Thermoelectric Properties of Polythiophenes by Their Chemical Structures and Doping Levels2017

    • Author(s)
      I. Imae, T. Koumoto, R. Akazawa, Y. Harima
    • Organizer
      2017 International Conference on Thermoelectrics
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Patent(Industrial Property Rights)] Thermoelectric conversion material and its manufacturing method2019

    • Inventor(s)
      I. Imae, Y. Harima, Y. Kataoka
    • Industrial Property Rights Holder
      I. Imae, Y. Harima, Y. Kataoka
    • Industrial Property Rights Type
      特許
    • Filing Date
      2019
    • Related Report
      2019 Annual Research Report
  • [Patent(Industrial Property Rights)] 熱電変換材料の製造方法、熱電変換素子の製造方法及び熱電変換材料の改質方法2019

    • Inventor(s)
      播磨裕,今栄一郎,櫻井康成,渡辺淳,後藤慶次
    • Industrial Property Rights Holder
      播磨裕,今栄一郎,櫻井康成,渡辺淳,後藤慶次
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2019-036599
    • Filing Date
      2019
    • Related Report
      2018 Research-status Report
  • [Patent(Industrial Property Rights)] 熱電変換材料の製造方法、熱電変換素子の製造方法及び熱電変換材料の改質方法2017

    • Inventor(s)
      播磨裕,今栄一郎,櫻井康成,渡辺淳,後藤慶次
    • Industrial Property Rights Holder
      播磨裕,今栄一郎,櫻井康成,渡辺淳,後藤慶次
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2017-155925
    • Filing Date
      2017
    • Related Report
      2017 Research-status Report

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

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