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Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift.

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Strain and geometry in palladium-copper (PdCu) alloys significantly alter electrochemical carbon dioxide reduction (CO2RR) pathways. Different local strain profiles dictate whether CO2 is converted to carbon monoxide (CO) or formate (HCOO-).

Keywords:
CO2 electroreductionPdCu alloyslocal strainpathway shift

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Understanding the electrochemical reduction of carbon dioxide (CO2RR) on bimetallic alloys is crucial for developing efficient catalysts.
  • Local microenvironment variables, including strain and geometric effects, complicate the prediction of CO2RR selectivity on Cu-based and Pd-based alloys.

Purpose of the Study:

  • To investigate how strain and geometric effects influence CO2RR selectivity on PdCu alloys.
  • To elucidate the specific adsorption geometries and reaction pathways of CO2 on PdCu nanoparticles and nanodendrites.

Main Methods:

  • Synthesis and characterization of PdCu nanoparticles and nanodendrites.
  • Electrochemical experiments to determine CO2RR selectivity.
  • In-situ spectroscopy to probe catalyst surface under reaction conditions.
  • Density functional theory (DFT) calculations to model adsorption energies and reaction pathways.

Main Results:

  • PdCu alloys with different geometries (nanoparticles vs. nanodendrites) exhibit distinct local strain profiles despite similar phases and facets.
  • CO2 preferentially adsorbs with carbon-side geometry on tensile-strained areas, favoring a *COOH-to-CO pathway.
  • CO2 adopts oxygen-side geometry on compressive-strained regions, promoting an *OCHO-to-HCOO pathway due to d-band center downshift.
  • Catalysts with both adsorption geometries show a dominant *OCHO-to-HCOO- pathway.

Conclusions:

  • Local strain environments in PdCu alloys are critical determinants of CO2RR selectivity.
  • Distinct geometric morphologies lead to varied local strain, influencing CO2 adsorption and subsequent reaction pathways.
  • This work provides a model for understanding bimetallic alloy microenvironments and their impact on CO2RR pathway shifts.