Citation: Weicheng Feng,  Jingcheng Yu,  Yilan Yang,  Yige Guo,  Geng Zou,  Xiaoju Liu,  Zhou Chen,  Kun Dong,  Yuefeng Song,  Guoxiong Wang,  Xinhe Bao. 调控双钙钛矿中高熵组分促进高温析氧反应[J]. Acta Physico-Chimica Sinica, ;2024, 40(6): 230601. doi: 10.3866/PKU.WHXB202306013 shu

调控双钙钛矿中高熵组分促进高温析氧反应

  • Corresponding author: Yuefeng Song,  Guoxiong Wang, 
  • Received Date: 5 June 2023
    Revised Date: 31 July 2023
    Accepted Date: 31 July 2023

    Fund Project: The project was supported by the National Key R&D Program of China (2021YFA1502400), the National Natural Science Foundation of China (22272176, 22002166, 22125205, 22072146, 22002158), the DNL Cooperation Fund, CAS (DNL202007), the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy (YLU-DNL Fund 2022008) and the CAS Youth Innovation Promotion (Y201938).

  • 固体氧化物电解池(SOEC)中阳极析氧反应动力学较为迟缓,限制了SOEC器件电催化转化能力,因此针对阳极材料的改性研究对于进一步提升SOEC电化学性能十分关键。高熵钙钛矿(HEP)在许多反应中表现出良好的催化活性,但在SOEC中的应用鲜有研究。本文通过在双钙钛矿的A位或A'位分别掺杂不同的稀土金属、碱土金属或碱金属离子,合成了(Pr0.2La0.2Sm0.2Nd0.2Gd0.2) BaCo2O6-δ(A-HEP)和Pr (Ba0.2Sr0.2Ca0.2Na0.2K0.2) Co2O6-δ(A'-HEP)两种高熵钙钛矿材料。由于掺杂离子平均半径和氧化态的差异,A-HEP保持四方双钙钛矿相结构而A'-HEP则转变为正交单钙钛矿相。物理化学表征结果表明,A-HEP中Co平均价态更高,Co 2p-O 1s杂化更强,从而增加了电子转移路径并降低了转移能垒。同时,A-HEP中表面氧空位浓度更高,可为阳极析氧反应提供更多的活性位点。因此,在具有A-HEP阳极的SOEC中,与氧输运、电子传输和表界面反应过程相关的阳极极化电阻显著降低,并在800℃下实现最高1.76 A·cm-2的电流密度和200 h的稳定性。本工作为高熵钙钛矿材料在SOEC阳极中的应用提供了新的策略。
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