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

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