CO 2 reduction on pure Cu produces only H 2 after subsurface O is depleted: Theory and experiment

• DOI: 10.1073/pnas.2012649118
• Publication Date: 2021-06-03T19:41:49Z
• Authors: Guiji Liu; Michelle Lee; Soonho Kwon; Guosong Zeng; Johanna Eichhorn; Aya K. Buckley; F. Dean Toste; William A. Goddard; Francesca M. Toma
• Keywords: 540; DFT; 01 natural sciences; 7. Clean energy; hydrogen evolution reaction; 0104 chemical sciences; Engineering; grand canonical potential kinetics; Nanotechnology; electrocatalysis; grand canonical potential; ethylene evolution

Significance

Electrochemical reduction of CO 2 to fuels and valuable chemicals is a global imperative to address energy and climate challenges. Despite enormous efforts, there is not yet a commercial process. The best catalyst remains Cu metal, but a great deal of controversy revolves around the role of the presence of oxygen in the material. We combine theory and experiments to show that pure Cu without subsurface oxygen leads to no organic products. Thus, maintaining substantial oxygen at Cu surfaces is essential for long-term reduction of CO 2 to organics.