Fan Xiaoxuan, Teng Zhenyuan, Han Lupeng, Shen Yongjie, Wang Xiyang, Qu Wenqiang, Song Jialing, Wang Zhenlin, Duan Haiyan, Wu Yimin A, Liu Bin, Zhang Dengsong
Innovation Institute of Carbon Neutrality, International Joint Laboratory of Catalytic Chemistry, State Key Laboratory of Advanced Special Steel, Department of Chemistry, College of Sciences, Shanghai University, Shanghai, China.
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, China.
Nat Commun. 2025 May 26;16(1):4874. doi: 10.1038/s41467-025-60043-6.
The electrochemical nitric oxide reduction reaction (NORR) holds a great potential for removing environmental pollutant NO and meanwhile generating high value-added ammonia (NH). Herein, we tactfully design and synthesize a ternary Co/CoO/CoB heterostructure that displays a high NH Faradaic efficiency of 98.8% in NORR with an NH yield rate of 462.18 µmol cm h (2.31 mol h g) at -0.5 V versus reversible hydrogen electrode, outperforming most of the reported NORR electrocatalysts to date. The superior NORR performance is attributed to the enhanced charge and proton transfer over the ternary Co/CoO/CoB heterostructure. The charge transfer between CoB and Co/CoO yields electron-deficient Co and electron-rich CoO. The electron-deficient Co sites boost HO dissociation to generate *H while the electron-rich low-coordination CoO sites promote NO adsorption. The *H formed on electron-deficient Co sites is more favorable to transfer to electron-rich CoO sites adsorbed with NO, facilitating the selective hydrogenation of NO. This study paves the way for designing and developing highly efficient electrocatalysts for electrochemical reduction of NO to NH.
电化学一氧化氮还原反应（NORR）在去除环境污染物NO并同时生成高附加值氨（NH₃）方面具有巨大潜力。在此，我们巧妙地设计并合成了一种三元Co/CoO/CoB异质结构，该结构在NORR中显示出98.8%的高NH₃法拉第效率，在相对于可逆氢电极-0.5 V时NH₃产率为462.18 μmol cm⁻² h⁻¹（2.31 mol h⁻¹ g⁻¹），优于迄今为止报道的大多数NORR电催化剂。优异的NORR性能归因于三元Co/CoO/CoB异质结构上增强的电荷和质子转移。CoB与Co/CoO之间的电荷转移产生缺电子的Co和富电子的CoO。缺电子的Co位点促进H₂O解离生成H，而富电子的低配位CoO位点促进NO吸附。在缺电子Co位点上形成的H更有利于转移到吸附有NO的富电子CoO位点，促进NO的选择性氢化。这项研究为设计和开发用于将NO电化学还原为NH₃的高效电催化剂铺平了道路。
