CO 2 electroreduction performance of PtS 2 supported single transition metal atoms: a theoretical study.

Electrocatalytic CO 2 reduction is a sustainable strategy to convert CO 2 into valuable carbon products. Atomically dispersed single-atom catalysts (SACs) have great potential as effective electrocatalysts for the CO 2 reduction reaction (CO 2 RR). Transition metal dichalcogenides (TMDs) are considered to be a kind of promising SAC supports. In this work, ten different 3d TM single atoms (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu and Zn) embedded in PtS 2 with single S-vacancy (TM-PtS 2 ) were designed by density functional theory (DFT) as candidate electrocatalysts for the CO 2 RR. Possible reaction pathways of CO 2 reduction to different C 1 products were systematically investigated. The results show that for all these TM-PtS 2 SACs, higher selectivity was achieved for CO 2 reduction to C 1 products than for the competing hydrogen evolution. HCOOH is the most favorable reduction product on PtS 2 -S v supported Sc, Ti, V, Cr, Mn, Fe and Cu SACs, while multiple C 1 products are generated on Co-, Ni- and Zn-PtS 2 . In particular, it is found that Sc-, V-, Fe-, Co- and Cu-PtS 2 exhibit higher electrocatalytic performance for the CO 2 RR than Cu(211). Therefore, these five SACs are promising CO 2 RR electrocatalysts.