Interfacial sp C–O–Mo Hybridization Originated High-Current Density Hydrogen Evolution

High-current density (≥1 A cm^-2) is a critical factor for large-scale industrial application of water-splitting electrocatalysts, especially seawater-splitting. However, it still remains a great challenge to reach high-current density due to the lack of active and stable intrinsic catalytic active sites in catalysts. Herein, we report an original three-dimensional self-supporting graphdiyne/molybdenum oxide (GDY/MoO₃) material for efficient hydrogen evolution reaction via a rational design of "sp C-O-Mo hybridization" on the interface. The "sp C-O-Mo hybridization" creates new intrinsic catalytic active sites (nonoxygen vacancy sites) and increases the amount of active sites (eight times higher than pure MoO₃). The "sp C-O-Mo hybridization" facilitates charge transfer and boosts the dissociation process of H₂O molecules, leading to outstanding HER activity with high-current density (>1.2 A cm^-2) in alkaline electrolyte and a decent activity and stability in natural seawater. Our results show that high-current density electrocatalysts can be achieved by interfacial chemical bond engineering, three-dimensional structure design, and hydrophilicity optimization.