法拉第效率
催化作用
选择性
硫黄
化学
再分配(选举)
氨生产
氧化还原
电化学
氮气
钼
无机化学
吸附
氨
可逆氢电极
电催化剂
二硫化钼
化学工程
电极
物理化学
有机化学
参比电极
政治
政治学
法学
工程类
作者
Lu Li,Weikang Yu,Wenbin Gong,Hao Wang,Chao‐Lung Chiang,Yanping Lin,Jie Zhao,Labao Zhang,Jong‐Min Lee,Guifu Zou
标识
DOI:10.1016/j.apcatb.2022.122038
摘要
Electrochemical nitrogen reduction reaction (NRR) is considered a sustainable approach that endows NH3 production from N2 and H2O under ambient conditions. Due to the sluggish adsorption/activation of N2 and the strong competition with the hydrogen evolution reaction, advanced NRR electrocatalysts with both high activity and selectivity are required. Herein, we demonstrate a local modulation strategy that simultaneously promotes NRR selectivity and activity on molybdenum-based single atom catalysts (SACs) by sulfur-induced electronic redistribution, delivering a NH3 yield rate of 46.6 μg·h−1·mgcat −1 and a Faradaic efficiency of 28.9% at a potential of − 0.2 V vs. RHE in 0.1 M HCl under ambient conditions. This study provides a promising strategy for synergizing the selectivity and activity of electrocatalysts toward multistep NRR. Moreover, such an atomic-level engineering strategy should be applicable to other SACs in general and may have a major impact on their use in electrocatalytic applications.
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