Electrocatalytic reduction of CO2 to alcohols would provide a synthetic sustainable way to convert renewable energy sources to transport fuels, however, large overpotentials and inability to control product selectivity are significant barriers to application. Recently, density functional theory (DFT) was used to evaluate the thermochemistry of CO2 electroreduction on various Cu surfaces, but questions about the preferred path remain. We report the first systematic DFT study to evaluate the elementary kinetics (i.e. activation barriers) for CO2 electroreduction on the Cu(111) surface. We find that CO reduction to COH or CHO intermediate is the key selectivity step for production of methane/ethylene over methanol. Our work provides a new path for CO2 electroreduction that matches recent electrokinetic experiments. Future work will focus on the effects of low-coordinated catalyst structures on CO2 electroreduction.

DFT studies of elementary kinetics of CO<sub>2</sub> reduction on Cu electrodes

245th National Meeting (2013)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.

DFT studies of elementary kinetics of CO2 reduction on Cu electrodes

DFT studies of elementary kinetics of CO₂ reduction on Cu electrodes