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Bimetallic effects on Zn-Cu electrocatalysts enhance activity and selectivity for the conversion of CO2 to CO

Wang, Lei and Peng, Hongjie and Lamaison, Sarah and Qi, Zhifu and Koshy, David M and Stevens, Michaela Burke and Wakerley, David and Zamora Zeledón, José A and King, Laurie A and Zhou, Lan and Lai, Yungchieh and Fontecave, Marc and Gregoire, John and Abild-Pedersen, Frank and Jaramillo, Thomas F and Hahn, Christopher (2021) Bimetallic effects on Zn-Cu electrocatalysts enhance activity and selectivity for the conversion of CO2 to CO. Chem Catalysis. ISSN 2667-1093

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Abstract

We report an active zinc-copper (Zn-Cu) bimetallic electrocatalyst for CO2 reduction to CO, prepared by a facile galvanic procedure. Under moderate overpotentials, Zn-Cu catalysts that are Zn rich exhibit intrinsic activity for CO formation superior to that of pure Zn, Cu, and Ag, the last of which is the state-of-the-art catalyst in CO2 electrolyzers. Combinatorial experiments involving catalysts prepared by physical vapor deposition reveal trends across the Zn-Cu system, corroborating the high CO selectivity unrivaled by other alloys and intermetallics. Physical and electrochemical characterization and first principles theory reveal that the origin of this synergy in intrinsic activity is an electronic effect from bimetallic Zn-Cu sites that stabilizes the carboxyl intermediate during CO2 reduction to CO. Furthermore, by integrating Zn-Cu into gas-diffusion electrodes, we demonstrate that bimetallic effects lead to improved electrocatalytic performance at industrially relevant currents. These insights provide catalyst design principles that can guide future development of efficient and earth-abundant CO-producing electrocatalysts.

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