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Promoting the OH cycle on an activated dynamic interface for electrocatalytic ammonia synthesis

Author

Listed:
  • Jiabao Lv

    (Zhejiang University
    Baima Lake Laboratory)

  • Ang Cao

    (Zhejiang University
    Technical University of Denmark)

  • Yunhao Zhong

    (Zhejiang University)

  • Qingyang Lin

    (Zhejiang University)

  • Xiaodong Li

    (Zhejiang University)

  • Hao Bin Wu

    (School of Materials Science and Engineering, Zhejiang University)

  • Jianhua Yan

    (Zhejiang University)

  • Angjian Wu

    (Zhejiang University
    Baima Lake Laboratory)

Abstract

Renewable-driven electrocatalytic nitrate conversion offers a promising alternative to alleviate nitrate pollution and simultaneously harvest green ammonia. However, due to the complex proton-electron transfer processes, the reaction mechanism remains elusive, thereby limiting energy efficiency. Here, we adopt Ni(OH)₂ as a model catalyst to investigate the dynamic evolution of the reaction interface. A proposed OH cycle mechanism involves the formation of a locally OH-enriched microenvironment to promote the hydrogenation process, which is identified through in-situ spectroscopy and isotopic labelling. By further activating the dynamic state through the implementation of surface vacancies via plasma, we achieve a high Faradaic efficiency of almost 100%. The activated interface accelerates the OH cycle by enhancing dehydroxylation, water dissociation, and OH adsorption, thereby promoting nitrate electroreduction and inhibiting hydrogen evolution. We anticipate that rational activation of the dynamic interfacial state can facilitate electrocatalytic interface activity and improve reaction efficiency.

Suggested Citation

  • Jiabao Lv & Ang Cao & Yunhao Zhong & Qingyang Lin & Xiaodong Li & Hao Bin Wu & Jianhua Yan & Angjian Wu, 2024. "Promoting the OH cycle on an activated dynamic interface for electrocatalytic ammonia synthesis," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50988-5
    DOI: 10.1038/s41467-024-50988-5
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    1. Suzanne Z. Andersen & Viktor Čolić & Sungeun Yang & Jay A. Schwalbe & Adam C. Nielander & Joshua M. McEnaney & Kasper Enemark-Rasmussen & Jon G. Baker & Aayush R. Singh & Brian A. Rohr & Michael J. St, 2019. "Author Correction: A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements," Nature, Nature, vol. 574(7777), pages 5-5, October.
    2. Kefu Zhu & Shiqiang Wei & Hongwei Shou & Feiran Shen & Shuangming Chen & Pengjun Zhang & Changda Wang & Yuyang Cao & Xin Guo & Mi Luo & Hongjun Zhang & Bangjiao Ye & Xiaojun Wu & Lunhua He & Li Song, 2021. "Defect engineering on V2O3 cathode for long-cycling aqueous zinc metal batteries," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    3. Suzanne Z. Andersen & Viktor Čolić & Sungeun Yang & Jay A. Schwalbe & Adam C. Nielander & Joshua M. McEnaney & Kasper Enemark-Rasmussen & Jon G. Baker & Aayush R. Singh & Brian A. Rohr & Michael J. St, 2019. "A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements," Nature, Nature, vol. 570(7762), pages 504-508, June.
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