SiFeN₆-graphene: A promising dual-atom catalyst for enhanced CO₂-to-CH₄ conversion

The synergistic effects in heteronuclear dual-atom catalysts create opportunities for designing highly efficient catalysts. In this work, we theoretically designed a stable SiFeN6-graphene with excellent CO2 electroreduction performance. The complementary properties of Si and Fe in the Si-Fe dual-atom center result in enhanced CO2 adsorption and activation, as well as weakened binding strength of the critical intermediate( & lowast;)OH, compared to SiN3- and FeN3-graphene. A low onset potential of -0.60 V is predicted for selective conversion of CO2 to CH4, with moderate kinetic barriers (less than 0.66 eV) during the whole reaction, readily surmountable under experimental conditions. This study provides vital insights into the rational design of dual-atom electrocatalysts by exploiting synergistic interactions between strategically paired atoms.