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Nanocluster Surface Microenvironment Modulates Electrocatalytic CO2 Reduction.

Seungwoo Yoo1,2, Suhwan Yoo1,3, Guocheng Deng1,2

  • 1Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul, 08826, Republic of Korea.

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|December 19, 2023
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Summary
This summary is machine-generated.

Chemists created a novel silver nanocluster with a hydrophobic shell, significantly boosting electrochemical CO2 reduction (eCO2RR) activity and stability. This breakthrough offers molecular insights into catalyst design for efficient carbon capture and utilization.

Keywords:
Ag25 nanoclusterCO2 reductioncarbon monoxideinterfacial structurelocal hydrophobicity

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Electrochemical CO2 reduction (eCO2RR) performance is limited by catalyst-electrolyte interfaces.
  • Precise control over interfacial microenvironments is crucial for understanding and optimizing eCO2RR.

Purpose of the Study:

  • To synthesize and characterize a precisely structured silver nanocluster with a tailored organic shell.
  • To investigate the impact of interfacial hydrophobicity on eCO2RR activity and selectivity.

Main Methods:

  • Synthesis of a 25-atom silver nanocluster (Ag25) coated with 18 thiolate ligands.
  • Electrochemical testing in an H-cell and a gas-fed membrane electrode assembly.
  • Operando surface-enhanced infrared absorption spectroscopy (SEIRAS).
  • Theoretical simulations.

Main Results:

  • Hydrophobic Ag25 clusters showed significantly enhanced eCO2RR activity (FE_CO: 90.3%, j_CO up to -240 mA cm-2) compared to hydrophilic ones (FE_CO: 66.6%).
  • The hydrophobic cluster demonstrated stable operation for over 120 hours.
  • SEIRAS and simulations revealed ligand-induced alterations in water structure and CO intermediates, crucial for eCO2RR.

Conclusions:

  • Confined hydrophobicity at the catalyst-electrolyte interface is a key factor in enhancing eCO2RR.
  • Atomistic understanding of interfacial effects provides a pathway for designing advanced electrocatalysts.
  • This work offers mechanistic insights into optimizing CO2 reduction for potential applications.