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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Highly stable and Active Cu1 /CeO2 Single-Atom Catalyst for CO Oxidation: A DFT Study.

Lan Qin1, Yun-Qi Cui2, Tao-Li Deng1

  • 1School of Chemistry and Chemical Engineering, Anshun University, Anshun, 561000, China.

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry
|October 25, 2018
PubMed
Summary

Single copper atoms on cerium dioxide exhibit high stability and promising catalytic activity for carbon monoxide oxidation. This single-atom catalyst operates effectively via the Mars van Krevelen mechanism.

Keywords:
CO oxidationdensity functional calculationsheterogeneous catalysisreaction mechanismssingle-atom catalyst

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Area of Science:

  • Materials Science
  • Catalysis
  • Surface Chemistry

Background:

  • Single-atom catalysts (SACs) offer unique advantages in heterogeneous catalysis due to their maximum atom utilization efficiency.
  • Cerium dioxide (CeO2) is a widely studied support material known for its oxygen storage capacity and redox properties.
  • Understanding the stability and reactivity of single metal atoms on oxide supports is crucial for designing advanced catalysts.

Purpose of the Study:

  • To investigate the stability and carbon monoxide (CO) oxidation activity of single copper (Cu) atoms supported on CeO2 (111).
  • To elucidate the electronic structure and adsorption properties of CO on the Cu1/CeO2 system.
  • To determine the catalytic mechanism for CO oxidation over this single-atom catalyst.

Main Methods:

  • Density Functional Theory (DFT) simulations were employed to model the Cu1/CeO2 system.
  • Calculations included binding energy, diffusion activation energy, and electronic structure analysis.
  • Frequency analysis was used to interpret CO adsorption spectra.

Main Results:

  • The Cu1/CeO2 single-atom catalyst demonstrates high stability, evidenced by strong binding energy and high diffusion activation energy for Cu atoms.
  • Electronic structure analysis confirmed the formation of Cu+ cations due to electron transfer from CeO2 to Cu.
  • Frequency analysis correlated experimental Infrared (IR) bands with Cu+-carbonyl species, confirming CO adsorption site.

Conclusions:

  • The Cu1/CeO2 single-atom catalyst exhibits excellent stability and significant potential for CO oxidation.
  • The catalytic activity proceeds via the Mars van Krevelen mechanism, involving the redox properties of the CeO2 support.
  • This study provides fundamental insights into the structure-activity relationship of single-atom catalysts on oxide supports.