CO2 Electrolysis via Surface-Engineering Electrografted Pyridines on Silver Catalysts

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Abstract

The electrochemical reduction of carbon dioxide (CO2) to value-added materials has received considerable attention. Both bulk transition-metal catalysts and molecular catalysts affixed to conductive noncatalytic solid supports represent a promising approach toward the electroreduction of CO2. Here, we report a combined silver (Ag) and pyridine catalyst through a one-pot and irreversible electrografting process, which demonstrates the enhanced CO2conversion versus individual counterparts. We find that by tailoring the pyridine carbon chain length, a 200 mV shift in the onset potential is obtainable compared to the bare silver electrode. A 10-fold activity enhancement at -0.7 V vs reversible hydrogen electrode (RHE) is then observed with demonstratable higher partial current densities for CO, indicating that a cocatalytic effect is attainable through the integration of the two different catalytic structures. We extended the performance to a flow cell operating at 150 mA/cm2, demonstrating the approach's potential for substantial adaptation with various transition metals as supports and electrografted molecular cocatalysts.

Original languageEnglish
Pages (from-to)7862-7876
JournalACS Catalysis
Volume12
Issue number13
DOIs
Publication statusPublished - 2022

Keywords

  • carbon dioxide reduction
  • electrografting
  • heterogeneous electrocatalysts
  • pyridine catalysts
  • silver electrocatalyst

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