Ma Chaoqun, Zhang Huaifang, Xia Jing, Zhu Xiaojuan, Qu Kaiyu, Feng Fukai, Han Sumei, He Caihong, Ma Xiao, Lin Gang, Cao Wenbin, Meng Xiangmin, Zhu Lijie, Yu Yifu, Wang An-Liang, Lu Qipeng
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China.
Shunde Innovation School, University of Science and Technology Beijing, Foshan 528399, China.
J Am Chem Soc. 2024 Jul 24;146(29):20069-20079. doi: 10.1021/jacs.4c04023. Epub 2024 Jul 10.
Electrocatalytic nitrate (NO) reduction reaction (NORR) holds great potential for the conversion of NO contaminants into valuable NH in a sustainable method. Unfortunately, the nonequilibrium adsorption of intermediates and sluggish multielectron transfer have detrimental impacts on the electrocatalytic performance of the NORR, posing obstacles to its practical application. Herein, we initially screen the adsorption energies of three key intermediates, i.e., *NO, *NO, and *HO, along with the d-band centers on 21 types of transition metal (IIIV and IB)-Sb/Bi-based intermetallic compounds (IMCs) as electrocatalysts. The results reveal that hexagonal CoSb IMCs possess the optimal adsorption equilibrium for key intermediates and exhibit outstanding electrocatalytic NORR performance with a Faradaic efficiency of 96.3%, a NH selectivity of 89.1%, and excellent stability, surpassing the majority of recently reported NORR electrocatalysts. Moreover, the integration of CoSb IMCs/C into a novel Zn-NO battery results in a high power density of 11.88 mW cm.
电催化硝酸盐（NO）还原反应（NORR）具有巨大潜力，可将NO污染物以可持续的方式转化为有价值的NH。不幸的是，中间体的非平衡吸附和缓慢的多电子转移对NORR的电催化性能有不利影响，为其实际应用带来了障碍。在此，我们首先筛选了三种关键中间体，即*NO、NO和HO的吸附能，以及21种过渡金属（IIIV和IB）-Sb/Bi基金属间化合物（IMCs）作为电催化剂的d带中心。结果表明，六方CoSb IMCs对关键中间体具有最佳的吸附平衡，并表现出出色的电催化NORR性能，法拉第效率为96.3%，NH选择性为89.1%，且稳定性优异，超过了大多数最近报道的NORR电催化剂。此外，将CoSb IMCs/C集成到新型Zn-NO电池中，可实现11.88 mW cm的高功率密度。
