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Self-Optimization With Oriented Facet Reconstruction for Universal Electrocatalytic C-N Coupling.

Ze Wu1, Xiaorong Zhu2, Xupeng Qin3

  • 1State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, International Joint Laboratory of Energy Electrochemistry Hunan University, Changsha, China.

Angewandte Chemie (International Ed. in English)
|June 9, 2026
PubMed
Summary
This summary is machine-generated.

Copper catalysts preferentially evolve to the highly active (111) facet during electrocatalytic C-N coupling, significantly boosting urea production from CO2 and nitrate. This facet engineering enhances catalyst performance and stability for green synthesis.

Keywords:
C–N couplingelectrocatalysisoriented facet reconstructionself‐optimizationsingle‐crystal

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis
  • Green Chemistry

Background:

  • Electrocatalytic carbon-nitrogen (C-N) coupling is a promising green synthesis route.
  • Understanding dynamic catalyst surface evolution is crucial for optimizing C-N coupling reactions.
  • Copper (Cu) catalysts are widely explored for C-N coupling, but their surface behavior is not fully elucidated.

Purpose of the Study:

  • To investigate the dynamic surface evolution of copper single crystals during nitrate-dominated electrocatalytic C-N coupling.
  • To understand how facet orientation influences catalytic activity and stability in C-N coupling.
  • To elucidate the mechanisms behind facet reconstruction and its impact on urea synthesis.

Main Methods:

  • Electrocatalytic experiments using Cu single crystals with different facets ((111), (110), (100)).
  • Synthesis of urea from carbon dioxide (CO2) and nitrate (NO3-) under electrochemical conditions.
  • Experimental and theoretical analyses (e.g., DFT) to study facet evolution and reaction mechanisms.

Main Results:

  • Observed preferential facet evolution on Cu single crystals, directing less active (110) and (100) facets towards the highly active (111) configuration.
  • The Cu(111) surface achieved a urea yield of 5.2 mg h⁻¹ cm⁻², significantly outperforming Cu(110) (4-fold) and Cu(100) (26-fold).
  • Facet reconstruction is driven by the chemical interaction between nitrate and copper, favoring the thermodynamically stable Cu(111) facet.

Conclusions:

  • The Cu(111) facet exhibits intrinsic catalytic superiority for nitrate-dominated C-N coupling.
  • Nitrate-driven facet reconstruction enhances electrocatalyst performance and stability.
  • This study advances the design principles for dynamically active electrocatalysts in green synthesis applications.