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 郭恒 于波 刘娟 李林秋 伍浩然 田维俊 张凤英 周莹

引用本文: 唐顺逸, 郭恒, 于波, 刘娟, 李林秋, 伍浩然, 田维俊, 张凤英, 周莹. 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[J]. 物理化学学报, 2026, 42(10): 100299. doi: 10.1016/j.actphy.2026.100299 shu
Citation:  Shunyi Tang,  Heng Guo,  Bo Yu,  Juan Liu,  Linqiu Li,  Haoran Wu,  Weijun Tian,  Fengying Zhang,  Ying Zhou. Hydrogen shuttle relay on Pd-Ru dual sites for high-efficiency nitrate electroreduction to ammonia[J]. Acta Physico-Chimica Sinica, 2026, 42(10): 100299. doi: 10.1016/j.actphy.2026.100299 shu

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

    通讯作者: 郭恒,E-mail:heng.guo@swpu.edu.cn; 周莹,E-mail:yzhou@swpu.edu.cn
  • 基金项目:

    四川省国际科技创新合作项目(2024YFHZ0303)、人力资源和社会保障部国家外国专家项目(H20240048)、成都市国际科技创新合作项目(2025-GH02-00034-HZ)和天府永兴实验室重大专项(2023KJGG15)。

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。

English

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  • 收稿日期:  2026-01-18
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