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

Jiabao Lv, Ang Cao, Yunhao Zhong, Qingyang Lin, Xiaodong Li, Hao Bin Wu (), Jianhua Yan () and Angjian Wu ()
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Jiabao Lv: Zhejiang University
Ang Cao: Zhejiang University
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

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-50988-5

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