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Catalysis02:50

Catalysis

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Updated: Aug 9, 2025

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Catalyst Aggregation Matters for Immobilized Molecular CO2RR Electrocatalysts.

Shaoxuan Ren1, Eric W Lees2, Camden Hunt3

  • 1Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada.

Journal of the American Chemical Society
|February 17, 2023
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Catalyst aggregation significantly impacts the performance of molecular electrocatalysts for carbon dioxide reduction (CO2RR). Dispersing catalysts on supports is crucial for accurate data and developing efficient, stable electrocatalysts for CO2RR.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Immobilized molecular electrocatalysts are key for carbon dioxide reduction reaction (CO2RR).
  • Catalyst aggregation can significantly alter the observed performance and mechanistic understanding of CO2RR.

Purpose of the Study:

  • To investigate the effect of catalyst aggregation on the behavior of immobilized cobalt phthalocyanine (CoPc) during CO2RR.
  • To develop strategies for engineering improved molecular electrocatalysts for CO2RR in flow cells.

Main Methods:

  • Utilized *operando* Raman spectroscopy to study CO2RR on immobilized CoPc in an electrochemical flow reactor.
  • Analyzed the influence of catalyst aggregation on CoPc oxidation state and catalytic activity.

Main Results:

  • Demonstrated that CoPc oxidation state during electrolysis depends on aggregation.
  • Showed that dispersed catalysts on conductive supports are essential for reliable CO2RR performance data.
  • Engineered an improved catalyst, EtO8-CoPc, achieving high selectivity (≥95% FE_CO), current density (≥300 mA/cm2), and durability.

Conclusions:

  • Accurate identification of active species in molecular catalysts requires *operando* spectroscopy and consideration of aggregation.
  • Dispersed molecular catalysts are vital for efficient CO2RR in flow cells.
  • The metal center of CoPc is the active site for CO2RR catalysis in flow cells.