Abstract
Electrochemical water splitting offers a most promising pathway for "green hydrogen" generation. Even so, it remains a struggle to improve the electrocatalytic performance of non-noble metal catalysts, especially bifunctional electrocatalysts. Herein, aiming to accelerate the hydrogen and oxygen evolution reactions, an oxygen-bridged cobalt-chromium (Co-O-Cr) dual-sites catalyst anchored on cobalt phosphide synthesized through MOF-mediation are proposed. By utilizing the filling characteristics of 3d orbitals and modulated local electronic structure of the catalytic active site, the well-designed catalyst requires only an external voltage of 1.53 V to deliver the current density of 20 mA cm(-2) during the process of water splitting apart from the superb HER and OER activity with a low overpotential of 87 and 203 mV at a current density of 10 mA cm(-2) , respectively. Moreover, density functional theory (DFT) calculations are utilized to unravel mechanistic investigations, including the accelerated adsorption and dissociation process of H(2) O on the Co-O-Cr moiety surface, the down-shifted d-band center, a lowered energy barrier for the OER and so on. This work offers a design direction for optimizing catalytic activity toward energy conversion.