Chapter 4: Single-crystal Surfaces as Model Electrocatalysts for CO₂ Reduction

Single-crystal electrodes have been essential in the development of fundamental understanding of complex catalytic reactions. Each facet of a single crystal provides a different reactivity and ability to bind intermediates, and pioneering work by Clavillier opened up the field for quantitative mechanistic study. This single-crystal work has now been performed for many types of metal surfaces and systematic studies as a function of crystal facets have been linked to computational electrochemistry to provide predictive tools and better insight into complex reaction sequences. This chapter summarises recent progress in, and current understanding of, carbon dioxide reduction reaction (CO₂RR) on a single-crystal electrode surface.