Designing TM-N2O2Cx single-atom catalysts for electrocatalytic CO2 reduction

Electrocatalytic CO2 reduction reaction (CO2RR) has been extensively considered as a potential carbon cycle technology because it can use CO2 as resources to produce high value-added fuels and chemicals under mild conditions. Therefore, developing highly efficient CO2RR catalysts is extremely significant. Here, we designed a series of TM-N2O2Cx (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn) single-atom catalysts and investigated their catalytic activities for CO2RR by using the density functional theory. Interestingly, these TM-N2O2Cx catalysts exhibit excellent CO2RR selectivity towards three kinds of different products, including CH4, CO, and HCOOH at relatively low overpotentials, where the CO2RR product of Sc-N2O2Cx, Mn-N2O2Cx, and Zn-N2O2Cx is CO, and that of V-N2O2Cx is CH4, while the other six catalysts would produce HCOOH. Moreover, the best pathway for CH4 formation is also unveiled, that is, * + CO2? C*OOH? C*O + H2O ? C*HO ? C*HOH? C*H + H2O ? C*H-2 ? C*H-3 ? * + CH4. In short, TM-N2O2Cx catalysts exhibit high catalytic activity for electrocatalytic CO2RR, which provides useful information for experimental scientists to synthesize these promising CO2RR catalysts.

Automated summary

In this study, a series of TM-N2O2Cx (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn) single-atom catalysts were designed and their catalytic activities for CO2RR were investigated using density functional theory. The results showed that these catalysts exhibited excellent selectivity towards three different CO2RR products, including CH4, CO, and HCOOH at relatively low overpotentials. The CO2RR products of Sc-N2O2Cx, Mn-N2O2Cx, and Zn-N2O2Cx were CO, while V-N2O2Cx produced CH4, and the other six catalysts produced HCOOH. Moreover, the best pathway for CH4 formation was also revealed. These TM-N2O2Cx catalysts demonstrated high catalytic activity for electrocatalytic CO2RR, providing useful information for the synthesis of promising CO2RR catalysts by experimental scientists.