Electrochemical Reduction of Gaseous Nitrogen Oxides on Transition Metals at Ambient Conditions. 2022

Byung Hee Ko, and Bjorn Hasa, and Haeun Shin, and Yaran Zhao, and Feng Jiao
Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, Delaware 19716, United States.

Mitigating nitrogen oxide (NO) emissions is critical to tackle global warming and improve air quality. Conventional NO abatement technologies for emission control suffer from a low efficiency at near ambient temperatures. Herein, we show an electrochemical pathway to reduce gaseous NO that can be conducted at high reaction rates (400 mA cm-2) 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 N2 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 NO emissions at ambient conditions by using renewable electricity.

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