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Ruperto G Mariano1, Kim McKelvey2, Henry S White2

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Grain boundaries in gold electrodes enhance catalytic activity for carbon dioxide reduction but not hydrogen evolution. This study provides direct evidence for exploiting grain boundary effects in heterogeneous catalysis.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Identifying active surfaces is crucial for tuning material catalytic properties.
  • Grain boundaries in polycrystalline materials can create high-energy, strained surfaces.
  • Previous correlations between grain boundary density and catalytic activity lack direct evidence.

Purpose of the Study:

  • To provide direct evidence that grain boundaries create catalytically active surfaces.
  • To investigate the role of grain boundaries in electrochemical carbon dioxide reduction and hydrogen evolution.
  • To correlate catalytic activity with the strain field at grain boundaries.

Main Methods:

  • Utilized bulk electrochemical measurements.
  • Employed scanning electrochemical cell microscopy with submicrometer resolution.
  • Examined gold electrodes to analyze grain boundary and grain surface activity.

Main Results:

  • Demonstrated that grain boundary surface terminations in gold are more active for electrochemical carbon dioxide (CO2) reduction to carbon monoxide (CO).
  • Showed that grain boundaries are not more active for the competing hydrogen (H2) evolution reaction.
  • Found the catalytic footprint of grain boundaries aligns with their dislocation-induced strain field.

Conclusions:

  • Grain boundaries act as active sites for specific catalytic reactions like CO2 reduction.
  • The catalytic activity is linked to the strain field generated by dislocations at grain boundaries.
  • This research offers a strategy for utilizing grain boundary effects in heterogeneous catalysis.