Substantial progress in enhancing the activity in electrochemical CO(2) reduction (eCO(2)RR) on Cu by optimizing reaction conditions and electrode setups has been made in the past two decades 1–3. However, an improvement of the intrinsic activity towards high value hydrocarbons could not be achieved1,2 since Hori et al.’s seminal work4. In order to enable such an enhancement, an understanding of the reaction mechanism on an atomistic scale is needed. In our talk, we will present density functional theory-based studies on eCO(2)RR. Applying novel constant potential DFT approaches5,6 allows us to explicitly study the potential dependence of both coupled proton-electron transfer and potential sensitive surface reactions. We will discuss the role of the two competing elementary reactions towards eCO(2)RR products and their consequences on the potential and pH response of the reactions. Understanding the underlying reaction process enables us to define descriptors for finding improved Cu surfaces and paves the way for the discovery of possible alternatives to copper-based catalysts.

Understanding electrochemical CO(2) reduction on well-defined Cu surfaces and beyond

ACS Spring Meeting 2021

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