2024 AIChE Annual Meeting
(7c) Tuning Copper Catalyst with Yttrium and Palladium Dual-Atom Alloying Strategy for Enhanced Electrochemical Reduction of CO2 to C2 Oxygenates
Electrochemical reduction of carbon dioxide (CO2) to liquid C2+ oxygenates presents a promising avenue for mitigating greenhouse gas emissions and value-added chemical syntheses. Copper (Cu) has emerged as perhaps the most versatile catalyst platform for this transformation; however, its efficacy is hindered by the often-mediocre reaction yields. To begin, as a continuation of our previous single-atom alloy work for electrocatalytic applications, we found that single-atom Y1Cu alloy renders facile conversion of CO2 to CO, but the subsequent hydrogenation of CO to multi-carbon species is limited. Along the line, single-atom Pd1Cu shows no obvious benefits for CO2 activation, while the presence of the single-atom Pd promoted C-C coupling and oxygenate formations. As a step forward in this work adopting the dual-atom alloy strategy, the single-atom Y and Pd species in affinity on copper surfaces lead to much more advanced reactivity. At – 1.1 V vs. RHE, the dual-atom Y1Pd1Cu catalyst exhibits a total current density of 172 mA/cm2 and liquid products Faradaic efficiency (FE) of 72.2 %, clearly advantageous to its Cu-only parent catalyst (70 mA/cm2, 13.2 %) as well as the single-atom alloy predecessors: Pd1Cu (60 mA/cm2, 50.5 %) and Y1Cu (129 mA/cm2, 38.4 %). Our work demonstrates the efficacy of the dual-atom alloy strategy in designing electrocatalysts advanced to their monometallic and single-atom alloy counterparts.