CO2 Electrolysis via Surface-Engineering Electrografted Pyridines on Silver Catalysts

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 non-catalytic solid supports, represents a promising approach towards electroreduction of CO2. Here, we report a combined silver (Ag) and pyridine catalyst through a green and irreversible electrografting process, which demonstrates enhanced CO2 conversion versus the individual counterparts. We find 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 RHE is then observed with demonstratable higher partial current densities for CO indicating a co-catalytic effect is attainable through the integration of the two different catalytic structures. We extended performance to a flow cell operating at 150 mA/cm2, demonstrating the approach’s potential for substantial adaption with various transition metals as supports, and electrografted molecular co-catalysts.