Hai Yan, Li Xiaoman, Cao Yue, Wang Xinyan, Meng Linghu, Yang Yang, Luo Min
State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, School of chemistry and Chemical Engineering, Ningxia University, Yinchuan, Ningxia 750021, PR China.
ACS Appl Mater Interfaces. 2024 Mar 6;16(9):11431-11439. doi: 10.1021/acsami.3c16456. Epub 2024 Feb 21.
Ammonia (NH) plays a vital role in industrial and agricultural development. The electrocatalytic nitrate reduction reaction (eNORR) is an effective method to produce NH under environmental conditions but also requires considerably active and selective electrocatalysts. Herein, a copper foam was used as a conductive substrate for the electrode materials. Specifically, a Co metal-organic framework (Co-MOF) was in situ grown on the copper foam, etched, and calcined to form NiCoO@Cu nanosheets, which were used as cathode electrodes for the eNORR. In 0.1 M NaSO with 0.1 M NaNO electrolyte, NiCoO@Cu nanosheets realized an NH yield of 5940.73 μg h cm at -0.9 V vs reversible hydrogen electrode (RHE), with a Faradaic efficiency of 94.2% at -0.7 V vs RHE. After 33 h of the catalytic reaction, the selectivity of NH-N increased to 99.7%. The excellent electrocatalytic performance of NiCoO@Cu nanosheets was attributed to the apparent synergistic effect between the Ni atoms and the Co atoms of bimetallic materials. This study shows that the Ni doping of NiCoO@Cu nanosheets effectively facilitated the adsorption of NO on NiCoO@Cu, and it promoted the eNORR.
氨(NH₃)在工农业发展中起着至关重要的作用。电催化硝酸盐还原反应(eNORR)是在环境条件下生产NH₃的有效方法,但也需要具有相当活性和选择性的电催化剂。在此,泡沫铜被用作电极材料的导电基底。具体而言,在泡沫铜上原位生长、蚀刻并煅烧钴金属有机框架(Co-MOF)以形成NiCoO₂@Cu纳米片,其用作eNORR的阴极电极。在含有0.1 M NaNO₃的0.1 M Na₂SO₄电解质中,NiCoO₂@Cu纳米片在相对于可逆氢电极(RHE)为-0.9 V时实现了5940.73 μg h⁻¹ cm⁻²的NH₃产率,在相对于RHE为-0.7 V时法拉第效率为94.2%。催化反应33小时后,NH₃-N的选择性提高到99.7%。NiCoO₂@Cu纳米片优异的电催化性能归因于双金属材料中Ni原子和Co原子之间明显的协同效应。该研究表明,NiCoO₂@Cu纳米片的Ni掺杂有效地促进了NO在NiCoO₂@Cu上的吸附,并促进了eNORR。