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Rectifying Heterointerface Facilitated C-N Coupling Dynamics Enables Efficient Urea Electrosynthesis Under Ultralow

Mingyu Cheng1, Shao Wang1, Zechuan Dai1

  • 1Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, 230026, Hefei, Anhui, P R. China.

Angewandte Chemie (International Ed. in English)
|September 25, 2024
PubMed
Summary

This study introduces a novel Cu/Cu2O catalyst for sustainable urea synthesis from CO2 and nitrate. The catalyst enhances urea yield and efficiency via nanoscale rectifying heterointerfaces, offering a greener alternative to traditional methods.

Keywords:
CuC−N couplingelectrocatalysisrectifying heterointerfaceurea electrosynthesis

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Sustainable Chemistry

Background:

  • Traditional urea synthesis (Bosch-Meiser method) is energy-intensive.
  • Electrocatalytic urea synthesis from CO2 and nitrate is a sustainable alternative.
  • Improving urea yield and Faradaic efficiency (FE) simultaneously is challenging due to complex intermediates.

Purpose of the Study:

  • To develop an efficient electrocatalyst for urea synthesis from CO2 and nitrate.
  • To investigate the role of catalyst nanostructure and interfaces in enhancing urea synthesis.
  • To provide insights into the reaction mechanism for improved C-N coupling.

Main Methods:

  • Fabrication of Cu/Cu2O Mott-Schottky catalyst with nanoscale rectifying heterointerfaces via in situ electroreduction of Cu2O nanowires.
  • Electrochemical characterization across ultralow applied potentials (0 to -0.3 V vs. RHE).
  • Operando synchrotron radiation-Fourier transform infrared spectroscopy (SR-FTIR) and density functional theory (DFT) calculations to study reaction intermediates and mechanisms.

Main Results:

  • Achieved notable FE (32.6-47.0%) and substantial urea yields (6.08-30.4 μmol h-1 cm-2).
  • Demonstrated catalyst performance across a broad range of ultralow applied potentials.
  • Confirmed the formation of *CO intermediates and C-N bonds using SR-FTIR.
  • DFT calculations revealed that the Cu/Cu2O heterointerface modulates *CO adsorption, enhancing C-N coupling dynamics.

Conclusions:

  • The developed Cu/Cu2O Mott-Schottky catalyst with nanoscale rectifying heterointerfaces offers a groundbreaking pathway for efficient electrocatalytic urea synthesis.
  • The study provides deep insights into copper-based heterointerface catalysts for C-N coupling and urea production.
  • This approach presents a sustainable and advanced method for synthesizing urea from CO2 and nitrate.