Efficient Electrochemical Nitrate Reduction to Ammonia Driven by a Few Nanometer-Confined Built-In Electric Field

纳米 电化学 硝酸盐 还原(数学) 电场 氨生产 材料科学 催化作用 纳米技术 无机化学 环境科学 化学 电极 物理 复合材料 有机化学 物理化学 数学 量子力学 几何学
作者
Maolin Zhang,Zedong Zhang,Shaolong Zhang,Zechao Zhuang,Kepeng Song,Karthik Paramaiah,Moyu Yi,Hao Huang,Dingsheng Wang
出处
期刊:ACS Catalysis 卷期号:: 10437-10446
标识
DOI:10.1021/acscatal.4c02317
摘要

Converting nitrate (NO3–) to ammonia (NH3) through the electrochemical reduction method offers an appealing approach for wastewater treatment and facilitates nitrogen cycling in nature. However, this electrolytic method involves a series of proton-coupled electron transfer processes and comes with severe competing reactions. Consequently, there is a significant demand for catalysts exhibiting good catalytic activities and selectivities. Here, a series of copper–cobalt binary sulfide nanosheets with varying Cu/Co compositions were prepared to investigate the synergy effects between the components copper sulfide and cobalt sulfide on their catalytic performance. As a result, a volcano-like correlation between the Cu/Co ratio and electrocatalytic performance was built. The optimal catalyst CuxS–Co0.5 exhibited a maximum Faradaic efficiency (FE) of ∼95.6% for ammonia at −1.4 V vs Ag/AgCl. The highest ammonia yield rate of 5.36 mg/h·cm2 was achieved at −1.6 V vs Ag/AgCl, which was 6.5- and 3.8-fold relative to those of pure CuxS and CoS2, respectively. By combining spectroscopy characterizations with theoretical calculations, we revealed that catalyst CuxS–Co0.5 with a built-in electric field confined to a few nanometers played a critical role in enhancing electron transfer and creating more active sites. Besides, its improved water dissociation capability was essential for the hydrogenation of reduction intermediates, collectively contributing to the enhanced catalytic performance.
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