物理化学学报 >> 2026, Vol. 42 >> Issue (10): 100299.doi: 10.1016/j.actphy.2026.100299

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基于氢穿梭接力的Pd-Ru双位点催化剂用于高效电还原硝酸盐制氨

唐顺逸1,2, 郭恒1,2,3,*(), 于波1,2, 刘娟1,2, 李林秋1,2, 伍浩然1,2, 田维俊1,2, 张凤英1,2,3, 周莹1,2,*()   

  1. 1 西南石油大学, 新能源与材料学院, 四川 成都 610500
    2 西南石油大学, 油气藏地质及开发工程全国重点实验室, 四川 成都 610500
    3 西南石油大学, 氢能绿色制储与高效利用川渝共建重点实验室, 四川 成都 610500
  • 收稿日期:2026-01-18 修回日期:2026-04-07 录用日期:2026-04-08 发布日期:2026-09-03
  • 通讯作者: Email: heng.guo@swpu.edu.cn (郭恒)yzhou@swpu.edu.cn (周莹)

Hydrogen shuttle relay on Pd-Ru dual sites for high-efficiency nitrate electroreduction to ammonia

Shunyi Tang1,2, Heng Guo1,2,3,*(), Bo Yu1,2, Juan Liu1,2, Linqiu Li1,2, Haoran Wu1,2, Weijun Tian1,2, Fengying Zhang1,2,3, Ying Zhou1,2,*()   

  1. 1 School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, Sichuan Province, China
    2 State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, Sichuan Province, China
    3 Sichuan-Chongqing Joint Key Laboratory of Green Hydrogen Production & Storage and Efficient Utilization, Southwest Petroleum University, Chengdu 610500, Sichuan Province, China
  • Received:2026-01-18 Revised:2026-04-07 Accepted:2026-04-08 Published:2026-09-03
  • Contact: Email: heng.guo@swpu.edu.cn (Heng Guo)yzhou@swpu.edu.cn (Ying Zhou)

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摘要：

电催化硝酸盐还原(NO3−RR)合成氨(NH3)为含硝酸盐工业废水资源化处理利用一体化提供了一条理想的路径。然而，该反应涉及多电子/质子转移步骤，在质子供应不足时动力学缓慢，导致氨选择性与产率低。本研究基于“氢穿梭接力”策略，设计了一种负载于镍泡沫(NF)上的Pd-Ru双金属催化剂(Pd-Ru/NF)，发现Pd位点主导硝酸盐活化与加氢过程，而Ru位点则高效裂解水分子产生活性氢物种(H*)。二者协同构成氢传递网络，实现反应位点间的氢溢流动态匹配，从而在加速硝酸盐加氢的同时，有效抑制析氢副反应(HER)。在−1.4 V (vs. RHE)电位下，Pd-Ru/NF催化剂的氨产率高达1.77 mmol cm−2 h−1，法拉第效率(FE)为85.95%。本工作通过构建双功能位点协同的氢接力机制，为设计高效NO3−RR催化剂提供了新范式。

关键词: 硝酸盐还原, 合成氨, 电催化, 金属负载

Abstract:

The electrocatalytic reduction of nitrate to ammonia (NO3−RR) represents a promising strategy for sustainable nitrogen cycling and the valorisation of wastewater. Its practical implementation, however, is limited by sluggish kinetics, stemming from inefficient proton delivery during the multi-step electron/proton transfer, which restricts both ammonia selectivity and yield. In this work, we report a Pd-Ru bimetallic catalyst supported on nickel foam (Pd-Ru/NF), which functions through a hydrogen shuttle relay mechanism between dual-function sites. Combined experimental and theoretical analyses indicate that Pd sites are principally responsible for nitrate activation and hydrogenation, while adjacent Ru sites efficiently cleave water to supply active hydrogen species (H*). This cooperative interaction creates a dynamic hydrogen-transfer network, enabling rapid and directed proton delivery to reaction intermediates. The relay process not only accelerates the critical hydrogenation steps but also effectively suppresses the competing hydrogen evolution reaction (HER). Consequently, the Pd-Ru/NF electrode attains a notable ammonia yield of 1.77 mmol cm−2 h−1 with a Faradaic efficiency of 85.95% at −1.4 V vs. RHE. This study establishes a novel catalyst design paradigm based on the management of interfacial hydrogen transfer, providing a general strategy to enhance the efficiency of proton-coupled electrocatalytic transformations.

Key words: Nitrate reduction, Ammonia synthesis, Electrocatalysis, Metal loading