Transition metal atoms embedded in monolayer C13N3 as OER/ORR bifunctional electrocatalysts†

Abstract

Developing bifunctional electrocatalysts for efficiently catalyzing the oxygen evolution/reduction reaction (OER/ORR) is essential for water electrolysis and other processes. Herein, we have investigated the OER and ORR performance of monolayered TM-C₁₃N₃ by first-principles calculations, where TM includes Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ag, Os, Ir, Pt, and Au. The results show that Pt-C₁₃N₃ has excellent bifunctional OER/ORR activity with overpotentials of 0.27 V for the OER and 0.39 V for the ORR. In addition, volcano plots and contour maps based on the linear relationship between the adsorption energies of oxygenated intermediates were established to characterize the OER/ORR activity trends of TM-C₁₃N₃. The origin of the OER/ORR activity is revealed by analyzing Bader charges, the d-band center, and the crystal orbital Hamiltonian population (COHP).