View article

The electrochemical reduction of CO2 is a promising technology to reach a carbon-neutral economy. However, among other challenges, the design of active and selective catalysts still limits such advances. Herein, we explored the atomistic engineering of the catalyst substrate as a strategy to tune Cu catalysts for CO2 reduction towards different C1 products by using generalized coordination numbers, GCN, as a structural descriptor of catalytic properties. We observed bifurcations on reaction mechanisms and significant changes in the predicted onset potentials, Uonset, towards CO, HCOOH, and CH4 as a function of the GCN values of the adsorption sites. For each product, we observed volcano plots of Uonset as a function of GCN that indicate activity peaks. We also compared the evolution of Uonset for different products to show that, regardless of the small Uonset values for CH4 on low-coordination sites, such …