Electrochemical Reduction of Gaseous Nitrogen Oxides on Transition Metals at Ambient Conditions

被引:168
作者
Ko, Byung Hee [1 ]
Hasa, Bjorn [1 ]
Shin, Haeun [1 ]
Zhao, Yaran [1 ]
Jiao, Feng [1 ]
机构
[1] Univ Delaware, Ctr Catalyt Sci & Technol, Dept Chem & Biomol Engn, Newark, DE 19716 USA
关键词
NITRIC-OXIDE; ELECTROREDUCTION; NOX; CATALYSTS; ABATEMENT; EXHAUST; PT(111);
D O I
10.1021/jacs.1c10535
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Mitigating nitrogen oxide (NOx) emissions is critical to tackle global warming and improve air quality. Conventional NOx abatement technologies for emission control suffer from a low efficiency at near ambient temperatures. Herein, we show an electrochemical pathway to reduce gaseous NOx that can be conducted at high reaction rates (400 mA cm(-1)) under ambient conditions. Various transition metals are evaluated for electrochemical reduction of NO and N2O to reveal the role of electrocatalyst in determining the product selectivity. Specifically, Cu is highly selective toward NH3 formation with >80% Faradaic efficiency in NO electroreduction. Furthermore, the partial pressure study of NO electroreduction revealed that a high NO coverage facilitates the N-N coupling reaction. In acidic electrolytes, the formation of NH3 is greatly favored, whereas the N-2 production is suppressed. Additional mechanistic studies were conducted by using flow electrochemical mass spectrometry to gain further insights into reaction pathways. This work provides a promising avenue toward abating gaseous NOx emissions at ambient conditions by using renewable electricity.
引用
收藏
页码:1258 / 1266
页数:9
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