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Structure-dependent CO2 reduction on molybdenite (MoS2) electrocatalysts.

Jake Limb1, Lachlan F Gaudin1, Cameron L Bentley1

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|April 11, 2024
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Scanning electrochemical cell microscopy revealed that defects on molybdenite (MoS2) electrocatalysts significantly enhance CO2 reduction reaction (eCO2RR) activity. This finding guides the design of efficient catalysts for CO2 electrolysis.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Electrochemical CO2 reduction (eCO2RR) is crucial for sustainable energy. Molybdenite (MoS2) shows promise as an earth-abundant electrocatalyst.
  • Understanding structure-activity relationships is key to optimizing eCO2RR performance.

Purpose of the Study:

  • To directly identify structure-dependent eCO2RR activity on MoS2 electrocatalysts.
  • To investigate the role of nanoscale defects in eCO2RR and hydrogen evolution reaction (HER).
  • To guide the rational design of advanced electrocatalysts for CO2 utilization.

Main Methods:

  • Utilized Scanning Electrochemical Cell Microscopy (SECCM) for nanoscale electrochemical analysis.
  • Employed an aqueous imidazolium-based aprotic ionic liquid electrolyte.
  • Compared electrochemical activity at defect sites (edge plane, EP) versus basal plane (BP) under CO2 and N2 atmospheres.

Main Results:

  • Nanoscale defects, particularly edge planes (EP), exhibit significantly higher overall electrochemical activity compared to the basal plane (BP).
  • Specific defects, such as step edges, show enhanced activity selectively under a CO2 atmosphere, indicating improved selectivity.
  • SECCM directly mapped the heterogeneous activity distribution on the MoS2 surface.

Conclusions:

  • Surface defects on MoS2 are critical active sites for eCO2RR.
  • Targeting and engineering these defects can enhance both activity and selectivity for CO2 reduction.
  • This study provides fundamental insights for designing efficient, earth-abundant electrocatalysts for large-scale CO2 electrolysis.