Using single-atom catalysts for the
electrochemical reduction of
carbon dioxide is a promising method for excess renewable electricity
as chemical energy in fuels. In this study, we have investigated single
non-noble metal atoms supported on nitrogen-doped graphene (M-N4@Gr, where M = Fe, Co, Ni) as catalysts for the electrocatalytic
reduction of CO2 using first-principles density functional
theory and the computational hydrogen electrode model. The results
show that HCOOH is the preferred product of CO2 reduction
on the Ni-N4@Gr catalyst with an overpotential of 1.511
V, while Fe-N4@Gr and Co-N4@Gr prefer to reduce
CO2 to CH4 with the overpotential of 0.877 and
0.687 V, respectively. The computational results revealed that the
coordination environment affects d orbital occupations, leading to
a difference in the spin polarization of the systems and thus affecting
the performance and selectivity of catalysts. Our work may pave the
way for extending single non-noble atom catalysts, which consist of
earth-abundant elements, toward electrocatalytic CO2 reduction
reaction by regulating coordination environments.
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