Self‐Optimization With Oriented Facet Reconstruction for Universal Electrocatalytic C–N Coupling
Abstract
ABSTRACT Electrocatalytic C–N coupling represents a green synthesis platform, yet the dynamic evolution of catalyst surfaces during the reaction remains poorly understood. Here, we report a nitrate‐dominated, preferential facet evolution on Cu single crystals that directs less active (110) and (100) facets toward the highly active (111) configuration. The Cu(111) surface delivers a urea yield of 5.2 mg h −1 cm −2 from CO 2 and NO 3 − , outperforming (110) and (100) by about 4‐ and 26‐fold, respectively, while maintaining excellent stability. Experimental and theoretical analyses reveal that this facet reconstruction is associated with spontaneous chemical interaction between nitrate and metallic copper, alongside the thermodynamic stability of the Cu(111) facet. Significantly, the pristine Cu(111) surface consistently outperforms Cu(110) and Cu(100), highlighting its intrinsic catalytic superiority. This work provides insights into nitrate‐dominated C–N coupling, advancing the design of dynamically active electrocatalysts.
Article Details
Authors (15)
Ze Wu
Xiaorong Zhu
Xupeng Qin
National Synchrotron Radiation Laboratory
Chu Zhang
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering
Nannan Guo
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University Urumqi China
Dawei Chen
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Advanced Catalytic Engineering Research Center of the Ministry of Education
Dafeng Yan
Hubei Key Laboratory for Precision Synthesis of Small Molecule Pharmaceuticals & Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, College of Chemistry and Chemical Engineering
Yujie Wang
Shenyang National Laboratory for Materials Science, Institute of Metal Research
Ruping Miao
State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Laboratory of Energy Electrochemistry Hunan University Changsha China
Kefan Zhang
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Advanced Catalytic Engineering Research Center of the Ministry of Education
Qinghua Liu
National Synchrotron Radiation Laboratory
Chade Lv
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering
Luxiang Wang
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University Urumqi China
Shuangyin Wang
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering
Chen Chen