Subsurface oxide plays a critical role in CO₂ activation by Cu(111) surfaces to form chemisorbed CO₂, the first step in reduction of CO₂.

ABSTRACT: A national priority is to convert CO₂ into high-value chemical products such as liquid fuels. Because current electrocatalysts are not adequate, we aim to discover new catalysts by obtaining a detailed understanding of the initial steps of CO₂ electroreduction on copper surfaces, the best current catalysts. Using ambient pressure X-ray photoelectron spectroscopy interpreted with quantum mechanical prediction of the structures and free energies, we show that the presence of a thin suboxide structure below the copper surface is essential to bind the CO₂ in the physisorbed configuration at 298 K, and we show that this suboxide is essential for converting to the chemisorbed CO₂ in the presence of water as the first step toward CO₂ reductio

SUBMITTER: Favaro M 

PROVIDER: S-EPMC5495248 | biostudies-literature | 2017 Jun

REPOSITORIES: biostudies-literature