Abstract
Scanning electrochemical cell microscopy (SECCM) is employed to directly identify the structure-dependent electrochemical CO2 reduction reaction (eCO2RR) activity of molybdenite (MoS2) electrocatalysts in an aqueous imidazolium-based aprotic ionic liquid electrolyte. Nanoscale defects, where the edge plane (EP) is exposed, are directly targeted, revealing heightened overall activity (eCO2RR + the competing hydrogen evolution reaction, HER) over the relatively inactive basal plane (BP). In addition, certain types of defects (e.g., step edges) only exhibit heightened activity under a CO2 atmosphere (i.e., compared to N2), indirectly confirming higher selectivity at these surface sites. Overall, this work will guide the bottom-up design of earth-abundant electrocatalysts for use in large-scale CO2 electrolysis.
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