Selective Conversion NOx Into Isoxazoles via Co–Zn Electrocatalyst Steering the Reaction Pathway
Abstract
ABSTRACT The electrocatalytic upcycling of NOx species into valuable N ‐heterocycles presents an attractive route, but it is challenged by complex paths and low catalytic activity. This work reports a highly selective strategy for the electrochemical reduction of NOx to isoxazoles via coupling with 1,3‐dicarbonyls, enabled by a Co–Zn dual‐atom catalyst (Co–Zn–NC). Interestingly, the system achieves a remarkable Faraday efficiency of 92% for isoxazole and significantly inhibits hydrogen and ammonia production. The unique electronic structure significantly regulates the energy barrier of nitrate reduction reaction and the hydrogen adsorption energy revealed by density functional theory calculations, while obtaining moderate affinity towards hydroxylamine intermediate and isoxazole product illustrated from the adsorption measurements. This strategy demonstrates exceptional universality across various nitrogen sources (NO 3 − , NO 2 − , NO, NO 2 ), carbon sources (1,3‐dicarbonyls), and a series of M–Zn–NC catalysts, establishing a novel paradigm for synthesizing structurally complex N─O heterocycles directly from inorganic nitrogen wastes and creating a new platform for sustainable molecular manufacturing.
Article Details
Authors (8)
Tao You
Hangzhou Institute of Advanced Studies, Zhejiang Normal University , 1108 Gengwen Road, Hangzhou, Zhejiang 311231,
Junyan Li
Department of Materials Science and Engineering
Shilin Bo
MOE Laboratory of Bioinorganic and Synthetic Chemistry GBRCE For Functional Molecular Engineering Lehn Institute of Functional Materials School of Chemistry Sun Yat‐Sen University Guangzhou China
Wenyu Yang
Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Chemistry for Energy Materials (2011-iChEM), College of Chemistry and Materials
Haixin Sun
Qinghua Liu
National Synchrotron Radiation Laboratory
Guangqin Li
MOE Laboratory of Bioinorganic and Synthetic Chemistry GBRCE For Functional Molecular Engineering Lehn Institute of Functional Materials School of Chemistry Sun Yat‐Sen University Guangzhou China
Li‐Zhu Wu
Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing China