Microkinetic Modelling of Electrochemical Oxygen Evolution Reaction on Ir(111)@N-Graphene Surface

We have explored the thermodynamics and microkinetic aspects of oxygen evolution catalysis on low loading of Ir(111) on nitrogen-doped graphene at constant potential. The electronic modification induced by N-doping is the reason for the reduced overpotential of OER. The N-induced defect in the charge density is observed with increasing charge-depleted region around the Ir atoms. The lattice contraction shifts the d-band center away from the Fermi level, which increases the barrier for OH* and O* formation on Ir(111) supported on NGr (Ir(111)@NGr). Thus, highly endothermic O* formation reduces the OOH* formation, which is the potential determining step. For comparison, all electronic and binding energy calculations were also performed against Ir NP supported on Gr (Ir(111)@Gr). The stepwise potential-dependent activation barrier ( $$ ) was obtained using the charge extrapolation method. The third step remains the RDS in all ranges of water oxidation potentials. The potential dependent $$ is further applied to the Eyring rate equation to obtain the current density ( $$ ) and correlation between $$ and pH dependence, i. e., OH^- concentration. The microkinetic $$ progression leads to a Tafel slope value of 30 mV dec^-1 at pH=14.0, requiring $$ .