ABSTRACT Utilizing electrochemical conversion of into hydrocarbons is envisioned as a strategy toward closing the carbon cycle in an effort to slow the anthropogenic climate change. The process, however, suffers from low energy efficiency and selectivity toward tailored products. To this day, success in producing significant amounts of multicarbon products is limited to a single catalyst, copper, complicating optimization on the catalyst side. In this paper, we present an ab initio screening of Cu‐free catalysts for the production of high value carbon products. In a sequential screening process, both intrinsic activity and catalyst stability have been investigated. This lead to the discovery of a series of alloys containing transition and post transition metals exhibiting promising activity together with stability against segregation. Selectivity against hydrogen production and oxidation tendencies are also screened, highlighting the need for caution regarding the latter at non‐reducing conditions. The performance of the selected catalysts is rationalized by systematic shifts in the transition metal d‐band centers through alloying, which can be applied as a guiding principle for the discovery of novel alloy catalysts. Based on this fundamental understanding, this work motivates experimental testing of predicted catalyst compositions and provides an intuitive rational for the prediction of further catalyst candidates.
Georg Kastlunger (Fri,) studied this question.