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Operando X-ray absorption spectroscopic investigation of electrocatalysts state in anion exchange membrane fuel cells

Author

Listed:
  • Qihao Li

    (Cornell University)

  • Christopher J. Pollock

    (Cornell University)

  • Joesene Soto

    (Cornell University
    Cornell University)

  • Andrés Molina Villarino

    (Cornell University)

  • Zixiao Shi

    (Cornell University)

  • Mihail R. Krumov

    (Cornell University)

  • David A. Muller

    (Cornell University
    Cornell University)

  • Héctor D. Abruña

    (Cornell University
    Cornell University)

Abstract

Capturing the active state of (electro)catalysts under operating conditions, namely operando, is the ultimate objective of (electro)catalyst characterization, enabling the unraveling of reaction mechanisms and advancing (electro)catalyst development. Operando insights advance our understanding of the correlations between electrochemical tests and device-level performances. However, operando characterization of electrocatalysts is challenging due to the complexity of electrochemical devices and instrumental limitations. As a result, the majority of electrocatalyst characterizations have been limited to half-cell in situ studies. Here, we present an operando X-ray absorption spectroscopic study of Mn spinel oxide electrocatalysts in an operating fuel cell employing a custom-designed cell. Our results reveal that in anion exchange membrane fuel cells, the Mn valence state, within spinel Mn3O4/C, increases to above 3+, adopting an octahedral coordination devoid of Jahn-Teller distortions. This structural change results in an AEMFC performance equivalent to that of Co1.5Mn1.5O4/C, a composition that outperforms Mn3O4/C in rotating disk electrode tests. Our results underscore the importance of operando characterizations in elucidating the active state of electrocatalysts and understanding the correlation(s) between electrochemical tests and device performance.

Suggested Citation

  • Qihao Li & Christopher J. Pollock & Joesene Soto & Andrés Molina Villarino & Zixiao Shi & Mihail R. Krumov & David A. Muller & Héctor D. Abruña, 2025. "Operando X-ray absorption spectroscopic investigation of electrocatalysts state in anion exchange membrane fuel cells," Nature Communications, Nature, vol. 16(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57177-y
    DOI: 10.1038/s41467-025-57177-y
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    References listed on IDEAS

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    1. David A. Cullen & K. C. Neyerlin & Rajesh K. Ahluwalia & Rangachary Mukundan & Karren L. More & Rodney L. Borup & Adam Z. Weber & Deborah J. Myers & Ahmet Kusoglu, 2021. "New roads and challenges for fuel cells in heavy-duty transportation," Nature Energy, Nature, vol. 6(5), pages 462-474, May.
    2. Kui Jiao & Jin Xuan & Qing Du & Zhiming Bao & Biao Xie & Bowen Wang & Yan Zhao & Linhao Fan & Huizhi Wang & Zhongjun Hou & Sen Huo & Nigel P. Brandon & Yan Yin & Michael D. Guiver, 2021. "Designing the next generation of proton-exchange membrane fuel cells," Nature, Nature, vol. 595(7867), pages 361-369, July.
    3. Ying Wang & Yao Yang & Shuangfeng Jia & Xiaoming Wang & Kangjie Lyu & Yanqiu Peng & He Zheng & Xing Wei & Huan Ren & Li Xiao & Jianbo Wang & David A. Muller & Héctor D. Abruña & Bing Joe Hwang & Junta, 2019. "Synergistic Mn-Co catalyst outperforms Pt on high-rate oxygen reduction for alkaline polymer electrolyte fuel cells," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
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