The exploration of earth-abundant and high-efficiency bifunctional electrocatalysts for overall water splitting is of vital importance for the future of hydrogen economy. Regulation of electronic structure through heteroatom-doping represents one of the most powerful strategies to boost the electrocatalytic performance of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, we report a rational design of O-incorporated CoP (denoted as O-CoP) nanosheets, which synergistically integrate the favorable thermodynamics through modification of electronic structures with accelerated kinetics through nanostructuring. Experimental results and density functional theory (DFT) simulations manifest that the appropriate O incorporation into CoP could dramatically modulate the electronic structure of CoP and alter the adsorption free energies of reaction intermediates, thus promoting the HER and OER activities. Specifically, the optimized O-CoP nanosheets exhibit efficient bifunctional performance in alkaline electrolyte, requiring overpotentials of 98 and 310 mV to deliver a current density of 10 mA cm<sup>-2</sup> for HER and OER, respectively. When served as bifunctional electrocatalysts for overall water splitting, a low cell voltage of 1.60 V is needed for achieving a current density of 10 mA cm<sup>-2</sup>. This proposed anion-doping strategy will bring new inspiration to boost the electrocatalytic performance of transition metal-based electrocatalysts for energy conversion applications.

Regulating the electronic structure of CoP nanosheets by O incorporation for high-efficiency electrochemical overall water splitting

ACS Spring Meeting 2021

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.