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Boosting CO2 Electrochemical Reduction with Atomically Precise Surface Modification on Gold Nanoclusters.

Site Li1,2, Anantha Venkataraman Nagarajan3, Dominic R Alfonso2

  • 1Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA, 15213, USA.

Angewandte Chemie (International Ed. in English)
|December 22, 2020
PubMed
Summary

Atomic modification of gold nanoclusters (NCs) with cadmium (Cd) significantly enhances electrochemical CO2 reduction. This Cd-doped Au19Cd2 catalyst shows superior selectivity and activity for converting CO2, offering a promising pathway for carbon capture technologies.

Keywords:
cadmiumcluster compoundsdopingreaction mechanismsreduction

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Area of Science:

  • Nanomaterials Science
  • Electrochemistry
  • Catalysis

Background:

  • Thiolate-protected gold nanoclusters (NCs) are explored as catalysts for the electrochemical carbon dioxide (CO2) reduction reaction (CO2 RR).
  • Optimizing NC structure is crucial for improving CO2 RR selectivity and activity.

Purpose of the Study:

  • To investigate the effect of atomic-level doping on the CO2 RR performance of gold nanoclusters.
  • To enhance the selectivity and activity of gold nanoclusters for the electrochemical CO2 reduction reaction through cadmium (Cd) substitution.

Main Methods:

  • Atomic-level modification of a Au23 nanocluster by substituting two surface gold (Au) atoms with cadmium (Cd) atoms, creating Au19Cd2.
  • Electrochemical evaluation of CO2 RR selectivity and activity.
  • Density-functional theory (DFT) calculations to elucidate reaction mechanisms and energy barriers.

Main Results:

  • Cd-doped Au19Cd2 exhibited enhanced CO2 RR selectivity (90-95%) at applied potentials between -0.5 to -0.9 V, doubling the performance of undoped Au23.
  • Au19Cd2 demonstrated the highest reported CO2 RR activity (2200 mA mg-1 at -1.0 V vs. RHE) among NCs.
  • DFT calculations revealed a lower thermodynamic energy barrier for CO formation (0.74 eV lower) on Au19Cd2 due to modified surface geometry and electronic structure.

Conclusions:

  • Atomic doping of Au NCs with Cd significantly boosts CO2 RR performance by altering surface properties and intermediate binding energies.
  • The synergistic effect between Au and Cd in NCs is a promising strategy for developing efficient electrocatalysts for CO2 conversion.
  • This study provides insights into the surface doping mechanism and bimetallic synergism in NC-based CO2 RR catalysis.