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Dynamic structural engineering of ferrocene-functionalized Ag20 nanoclusters for enhanced CO2 electroreduction

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We developed a novel silver nanocluster (Ag20-Fc) using organometallic ligands for enhanced CO2 reduction. This hybrid catalyst shows superior performance and stability in converting CO2 to CO.

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Area of Science:

  • Nanomaterials Science
  • Catalysis
  • Organometallic Chemistry

Background:

  • Hybrid catalysts combining organometallic motifs and metal nanoclusters offer tunable active sites.
  • Silver nanoclusters are promising for catalysis but require precise structural control.

Purpose of the Study:

  • To synthesize and characterize a novel silver nanocluster, Ag20-Fc, with a unique sandwich-like architecture.
  • To investigate the structure-activity relationship of Ag20-Fc in electrocatalytic CO2 reduction.
  • To elucidate the mechanism behind the enhanced catalytic performance.

Main Methods:

  • Cooperative coordination synthesis using thiacalix[4]arene (TC4A) and ferrocenylacetylene ligands.
  • Electrospray ionization mass spectrometry (ESI-MS) for structural analysis in solution.
  • Electrocatalytic CO2 reduction experiments and Density Functional Theory (DFT) calculations.

Main Results:

  • A sandwich-type Ag20-Fc nanocluster with a tunable structure was synthesized.
  • Ag20-Fc demonstrated excellent electrocatalytic CO2 reduction to CO with >98% Faradaic efficiency and 24h stability.
  • DFT calculations revealed that ferrocenyl group hybridization enhances catalytic activity by lowering the *COOH intermediate formation barrier.

Conclusions:

  • The Ag20-Fc nanocluster represents a significant advancement in hybrid catalyst design for CO2 electroreduction.
  • Ligand engineering and understanding the electronic structure are crucial for optimizing nanocluster catalysts.
  • This work provides a pathway for developing highly efficient and stable catalysts for carbon utilization.