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Development of efficient low-cost SOFC/SOEC protonic cathodes for reliable energy distribution

研究課題

研究課題/領域番号 19K05672
研究種目

基盤研究(C)

配分区分基金
応募区分一般
審査区分 小区分36020:エネルギー関連化学
研究機関九州大学

研究代表者

Kwati Leonard  九州大学, カーボンニュートラル・エネルギー国際研究所, 准教授 (70734391)

研究期間 (年度) 2019-04-01 – 2025-03-31
研究課題ステータス 交付 (2023年度)
配分額 *注記
4,420千円 (直接経費: 3,400千円、間接経費: 1,020千円)
2021年度: 910千円 (直接経費: 700千円、間接経費: 210千円)
2020年度: 1,690千円 (直接経費: 1,300千円、間接経費: 390千円)
2019年度: 1,820千円 (直接経費: 1,400千円、間接経費: 420千円)
キーワードProtonic defects / ionic transport / Triple conducting / Fuel cell / Catalytic activity / Electrolysis / proton kinetics / hydration / protonic air electrode / catalytic activity / steam electrolysis / fuel cell / mixed conductivity / Electrolysis cell / Air electrode / Ionic transport / protonic defects / air electrode / oxygen vacancies / protonic cathode / electrolysis cell / reliable energy / low cost / proton transport / robust air electrodes / Proton conductor / SOFC/SOEC / sustainable Energy
研究開始時の研究の概要

Development of efficient low-cost SOFC/SOEC protonic cathodes for reliable energy distribution. I will synthesize and evaluate, robust highly active mixed protonic /electronic conducting cathode materials for operation at 600 ~ 400 °C, by investigating the synergistic effect of co-doping niobium (Nb5+), tantalum (Ta5+) and/or Zn2+, Sc3+ on the B-site of cation-ordered double perovskite, in an effort to enhance hydrogen incorporation and to create channels for fast diffusion. Research these cathodes will improve cell reliability, reduce costs and expedite commercialization of SOFC/SOEC

研究実績の概要

Solid-oxide fuel cells and electrolyzers that conduct protons are promising green energy conversion and storage technologies suited for low to intermediate-temperature regimes (300 -600 oC). However, their commercial viability has been hindered, in part, by the positrode’s kinetics and effective catalytic activity toward oxygen reduction and evolution reactions (ORR/OER).
The origin of catalytic activity in LnCo0.5Ni0.5O3-δ (Ln=La, Pr and Nd) perovskites "positrodes" (positive electrode) by low energy-ion scattering (LEIS) and DFT studies were investigated. The results reveal that La, Pr, and Pr cations dominate the outer atomic layer, with profound implications for catalytic activity. On the other hand, first principle calculations performed using the plane-wave DFT method and hybrid HSE06 functional suggest that the catalytic activity and electronic properties depend on the valence shell structure of the Ln-site cation and their redox properties.
non-stoichiometric A-site defects were introduced into PrxCo0.5Ni0.5O3-δ oxides (x = 1, 0.95, 0.9) to tune their mixed conduction properties. Pr deficiency can alter the charge compensation mechanism, leading to additional oxygen vacancies, subsequently translating to enhanced protonic fuel cells and electrolysis performance. Pr0.95Co0.5Ni0.5O3-δ:BaZr0.16Ce0.64Y0.1Yb0.1O3-δ (ratio 80:20) air electrodes show the lowest polarization resistance (Rp) of ~0.22 cm-2 (at 600 °C), determined from fuel cell mode of operation.

現在までの達成度 (区分)
現在までの達成度 (区分)

2: おおむね順調に進展している

理由

Using some of the materials characterized above specifically Pr0.95Co0.5Ni0.5O3-δ:BaZr0.16Ce0.64Y0.1Yb0.1O3-δ (ratio 80:20) as the air electrode on my half-cell demonstrates remarkable capabilities and endurance within the 450-600°C temperature range, achieving a peak power density of 1.13 W cm-2 at 600 oC in the fuel cell mode and a high current density of 1.5 A cm-2 at 1.3 V in the electrolysis mode. Suggesting a better understanding of the air electrode materials

今後の研究の推進方策

In other to fully understand the underlying principles of ionic transport in protonic oxides, additional spectroscopic studies are required to reveal their electronic properties, the spin state of constituent cations, their coordination, and changes while the oxide is being exposed to water vapor. Going forward, I will focus on using X-ray absorption spectroscopy (XAS) realized in both near-edge and extended ranges (if possible) to further understand the dependence between elemental compositions and their electron configuration. Detailed near-edge feature analysis will be performed to obtain information on the oxidation state and changes in the electronic structure of all elements upon hydration.

報告書

(5件)
  • 2023 実施状況報告書
  • 2022 実施状況報告書
  • 2021 実施状況報告書
  • 2020 実施状況報告書
  • 2019 実施状況報告書
  • 研究成果

    (10件)

すべて 2023 2022 2020 2019 その他

すべて 雑誌論文 (2件) (うち国際共著 2件、 査読あり 2件) 学会発表 (7件) (うち国際学会 4件、 招待講演 2件) 備考 (1件)

  • [雑誌論文] Tailored and Improved Protonic Conductivity through Ba(ZxCe10-x)0.08Y0.2O3-δ Ceramics Perovskites Type Oxides for Electrochemical Devices2022

    • 著者名/発表者名
      Leonard Kwati、Okuyama Yuji、Ivanova Mariya E.、Meulenberg Wilhelm A.、Matsumoto Hiroshige
    • 雑誌名

      ChemElectroChem

      巻: 9 号: 4

    • DOI

      10.1002/celc.202101663

    • 関連する報告書
      2021 実施状況報告書
    • 査読あり / 国際共著
  • [雑誌論文] Anode Supported Planar 5 × 5 cm2 SrZr0.5Ce0.4Y0.1O2.95 Based Solid Oxide Protonic Fuel Cells via Sequential Tape-Casting2022

    • 著者名/発表者名
      Kwati Leonard, Mariya E. Ivanova, Andre Weber, Wendelin Deibert, Wilhelm A. Meulenberg, Tatsumi Ishihara, Hiroshige Matsumoto
    • 雑誌名

      Solid State Ionics

      巻: 379 ページ: 115918-115918

    • DOI

      10.1016/j.ssi.2022.115918

    • 関連する報告書
      2021 実施状況報告書
    • 査読あり / 国際共著
  • [学会発表] Triple Conducting Oxides as Positrodes for proton-conducting Solid Oxide Electrochemical Devices2023

    • 著者名/発表者名
      Kwati Leonard (PI)
    • 学会等名
      15th Pacific Rim Conference of Ceramic Societies (PACRIM15)
    • 関連する報告書
      2023 実施状況報告書
    • 国際学会 / 招待講演
  • [学会発表] Resolving the influence of Sr and Ni diffusion on the moderate-temperature sintering of BaZr0.44Ce0.36Y0.2O3/SrZr0.4Ce0.4Y0.1O3 NiO proton conducting half-cells2023

    • 著者名/発表者名
      Kwati Leonard (PI)
    • 学会等名
      電気化学会第91回大会
    • 関連する報告書
      2023 実施状況報告書
    • 招待講演
  • [学会発表] Understanding the Origin of Enhanced Catalytic Activity inLnCo0.5Ni0.5O3-δ (Ln = Pr, La) Perovskites Type Oxides on Protonic Electrochemical Device2022

    • 著者名/発表者名
      Kwati Leonard (PI)
    • 学会等名
      23rd International Conference on Solid State Ionics (SSI 23)
    • 関連する報告書
      2022 実施状況報告書
    • 国際学会
  • [学会発表] Investigating the Origin of Enhanced Catalytic Activity in LnCo0.5Ni0.5O3-δ (Ln = La, Pr, Nd) "Positrodes" on Ceramic Protonic electrolytes2022

    • 著者名/発表者名
      Kwati Leonard (PI)
    • 学会等名
      第48回 固体イオニクス討論会
    • 関連する報告書
      2022 実施状況報告書
    • 国際学会
  • [学会発表] Processing Ceramic Protonic Oxide Via Inverse Tape Casting for use in Electrochemical Devices2020

    • 著者名/発表者名
      KWATI Leonard
    • 学会等名
      第33回秋季シンポジウム 公益社団法人日本セラミックス協会
    • 関連する報告書
      2020 実施状況報告書
  • [学会発表] Layered Ceramic Protonic Electrolyzers Fabricated Via Inverse Tape Casting2020

    • 著者名/発表者名
      KWATI Leonard
    • 学会等名
      The Power of Interfaces: Fundamentals for Solid State Devices, London
    • 関連する報告書
      2019 実施状況報告書
    • 国際学会
  • [学会発表] Proton investigation in Mixed ionic/electronic Conducting Air Electrode Materials2019

    • 著者名/発表者名
      KWATI Leonard
    • 学会等名
      15th Solid State Ionic, Lake Biwa, Shiga Japan
    • 関連する報告書
      2019 実施状況報告書
  • [備考] the-power-of-interfaces

    • URL

      https://www.imperial.ac.uk/events/95807/the-power-of-interfaces-fundamentals-for-solid-state-devices/

    • 関連する報告書
      2019 実施状況報告書

URL: 

公開日: 2019-04-18   更新日: 2024-12-25  

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