Electron induction of atomically dispersed Fe sites by adjacent Te atoms promotes CO2 activation in electroreduction

We report an electron induction regulation mechanism of single-atomic Fe sites by adjacent Te atoms to construct Fe–Te diatomic sites (DASs) for synergistic electrocatalytic CO2 reduction reaction (CO2RR). The Fe–Te DASs feature stable and unique N3Fe–TeC3 structures, with low-valence Feδ+ binding with one C atom and one O atom of CO2, and the adjacent Teδ+ acts as an electron donor, adjusting the electronic structure of Feδ+ sites, and stabilizes another negative O atom of CO2 by favorable electrostatics, strengthening CO2 adsorption and activation. Notably, the catalyst delivers a high CO selectivity above 90% over a wide potential range and good stability. The formation of Fe–Te DASs elevates the Fermi level and strengthens the interaction of the 2 πu orbital of CO2, which is easier to bend and forms activated CO2 intermediate, thereby decreasing the activation barrier and promoting the CO2RR process.