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

文献类型： 外文期刊

作者： Zhang, Maolin 1 ; Zhang, Zedong 2 ; Zhang, Shaolong 3 ; Zhuang, Zechao 4 ; Song, Kepeng 5 ; Paramaiah, Karthik 6 ; Yi, Moyu 6 ; Huang, Hao 6 ; Wang, Dingsheng 2 ;

作者机构： 1.Chinese Acad Agr Sci, Inst Environm & Sustainable Dev Agr, Beijing 100081, Peoples R China

2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

3.Shenzhen Univ, Coll Chem & Environm Engn, Shenzhen 518060, Peoples R China

4.Columbia Univ, Dept Chem Engn, New York, NY 10027 USA

5.Shandong Univ, Electron Microscopy Ctr, Jinan 250100, Peoples R China

6.King Abdullah Univ Sci & Technol, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia

关键词： copper-cobalt binary sulfide nanosheets; built-inelectric field; synergetic effect; electrocatalysis; nitrate reduction

期刊名称：ACS CATALYSIS （ 影响因子：11.3； 五年影响因子：12.6 ）

ISSN： 2155-5435

年卷期： 2024 年 14 卷 14 期

页码：

收录情况： SCI

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-Co-0.5 exhibited a maximum Faradaic efficiency (FE) of similar to 95.6% for ammonia at -1.4 V vs Ag/AgCl. The highest ammonia yield rate of 5.36 mg/hcm(2) 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-Co-0.5 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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