Hydrogen shuttle relay via Ru-Cu dual sites for high-efficiency nitrate electroreduction to green ammonia

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Guo, Heng, Tian, Shiqi, Luo, Shumin, Wu, Haoran, Li, Tingsong, Chen, Guoxing, Tu, Xin ORCID: 0000-0002-6376-0897, Tian, Weijun, Tang, Chun, Yang, Guidong et al (show 1 more authors) and Zhou, Ying (2026) Hydrogen shuttle relay via Ru-Cu dual sites for high-efficiency nitrate electroreduction to green ammonia Applied Catalysis B: Environment and Energy, 381. p. 125865. ISSN 0926-3373

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Abstract

The electrocatalytic nitrate reduction reaction (NO<inf>3</inf>^-RR) offers a promising pathway for green ammonia synthesis, yet suffers from inefficient hydrogen utilization due to competing proton consumption pathways. Here, we engineer a Ru-Cu<inf>2</inf>O/Cu catalyst via cationic spatial confinement, where Ru incorporation induces a dynamic hydrogen shuttle relay between reaction active sites. In situ/operando characterization technologies and theoretical calculations reveal that Ru sites accelerate water dissociation kinetics, generating mobile H* species that shuttle between Ru and Cu<inf>2</inf>O to synchronize dual reaction pathways: H*-mediated nitrate hydrogenation and electron-driven NH<inf>x</inf> intermediate conversion. Crucially, this shuttle relay enables kinetic matching of H flux between NO<inf>3</inf>^-RR and hydrogen evolution reaction, suppressing parasitic H<inf>2</inf> evolution while achieving a Faradaic efficiency (FE) of 95.68 % with an NH<inf>3</inf> yield rate of 0.82 mmol cm⁻² h⁻¹ at −0.2 V vs. RHE—1.65-fold higher than Cu<inf>2</inf>O/Cu controls. In addition, the catalyst maintains initial activity after 50 cycles. This work promotes the multi-step electrochemical hydrogenation process in nitrate reduction to ammonia (NO<inf>3</inf>^-RR) by constructing an efficient hydrogen transport path.

Item Type:	Article
Uncontrolled Keywords:	4004 Chemical Engineering, 40 Engineering, 34 Chemical Sciences
Divisions:	Faculty of Science & Engineering Faculty of Science & Engineering > School of Engineering Faculty of Science & Engineering > School of Engineering > Electrical Engineering and Electronics
Depositing User:	Symplectic Admin
Date Deposited:	03 Nov 2025 08:21
Last Modified:	23 Dec 2025 01:51
DOI:	10.1016/j.apcatb.2025.125865
Related Websites:	Publisher
URI:	https://livrepository.liverpool.ac.uk/id/eprint/3195168
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