山东大学鲁启鹏团队报道了基于中间吸附平衡的电催化硝酸还原制氨金属间化合物筛选。相关研究成果于2024年7月10日发表在《美国化学会杂志》。

电催化硝酸盐（NO₃^-）还原反应（NO₃RR）在可持续的方法中将NO₃^-污染物转化为有价值的NH₃方面具有巨大的潜力。不幸的是，中间体的非平衡吸附和缓慢的多电子转移对NO₃RR的电催化性能产生了不利影响，阻碍了其实际应用。

该文中，研究人员首先筛选了三种关键中间体的吸附能，即*NO₃、*NO和*H₂O，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，并表现出优异的电催化NO₃RR性能，法拉第效率为96.3%，NH₃选择性为89.1%，稳定性优异，超过了最近报道的大多数NO₃RR电催化剂。此外，将CoSb IMC/C集成到新型Zn-NO₃^-电池中可获得11.88 mW cm^-2的高功率密度。

附：英文原文

Title: Screening of Intermetallic Compounds Based on Intermediate Adsorption Equilibrium for Electrocatalytic Nitrate Reduction to Ammonia

Author: Chaoqun Ma, Huaifang Zhang, Jing Xia, Xiaojuan Zhu, Kaiyu Qu, Fukai Feng, Sumei Han, Caihong He, Xiao Ma, Gang Lin, Wenbin Cao, Xiangmin Meng, Lijie Zhu, Yifu Yu, An-Liang Wang, Qipeng Lu

Issue&Volume: July 10, 2024

Abstract: Electrocatalytic nitrate (NO3–) reduction reaction (NO3RR) holds great potential for the conversion of NO3– contaminants into valuable NH3 in a sustainable method. Unfortunately, the nonequilibrium adsorption of intermediates and sluggish multielectron transfer have detrimental impacts on the electrocatalytic performance of the NO3RR, posing obstacles to its practical application. Herein, we initially screen the adsorption energies of three key intermediates, i.e., *NO3, *NO, and *H2O, 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 NO3RR performance with a Faradaic efficiency of 96.3%, a NH3 selectivity of 89.1%, and excellent stability, surpassing the majority of recently reported NO3RR electrocatalysts. Moreover, the integration of CoSb IMCs/C into a novel Zn-NO3– battery results in a high power density of 11.88 mW cm–2.

DOI: 10.1021/jacs.4c04023

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c04023