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)
(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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Text
ACB Revised manuscript.pdf - Author Accepted Manuscript Available under License Creative Commons Attribution. Download (1MB) | Preview |
Abstract
The electrocatalytic nitrate reduction reaction (NO<inf>3</inf><sup>-</sup>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><sup>-</sup>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<sup>−2</sup> h<sup>−1</sup> 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><sup>-</sup>RR) by constructing an efficient hydrogen transport path.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | 4004 Chemical Engineering, 40 Engineering, 34 Chemical Sciences, 7 Affordable and Clean Energy |
| 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: | 03 Nov 2025 08:21 |
| DOI: | 10.1016/j.apcatb.2025.125865 |
| Related Websites: | |
| URI: | https://livrepository.liverpool.ac.uk/id/eprint/3195168 |
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