Improved high-current-density hydrogen evolution reaction kinetics on single-atom Co embedded in an order pore-structured nitrogen assembly carbon support†

Abstract

Single-atom catalysis is a subcategory of heterogeneous catalysis with well-defined active sites. Numerous endeavors have been devoted to developing single-atom catalysts for industrially applicable catalysis, including the hydrogen evolution reaction (HER). High-current-density electrolyzers have been pursued for single-atom catalysts to increase active-site density and enhance mass transfer. Here, we reasoned that a single-atom metal embedded in nitrogen assembly carbon (NAC) catalysts with high single-atom density, large surface area, and ordered mesoporosity, could fulfil an industrially applicable HER. Among several different single-atom catalysts, the HER overpotential with the best performing Co-NAC reached a current density of 200 mA cm⁻² at 310 mV, which is relevant to industrially applicable current density. Density functional theory (DFT) calculations suggested feasible hydrogen binding on single-atom Co resulted in the promising HER activity over Co-NAC. The best-performing Co-NAC showed robust performance under alkaline conditions at a current density of 50 mA cm⁻² for 20 h in an H-cell and at a current density of 150 mA cm⁻² for 100 h in a flow cell.