Direct Hydrogen Energy Conversion on Industrial‐Current‐Density

ABSTRACT Realizing efficient hydrogen evolution reaction at an industrial scale and achieving high current density is of great significance for building a sustainable hydrogen energy system and is highly anticipated by both the scientific and industrial communities. The key to achieving this goal lies in developing a transformative catalytic system that can promote rapid and efficient hydrogen production at high current density. In this report, we propose a strategy to regulate the electrochemical environment and activation energy at the atomic level, enabling intelligent control of the surface charge distribution and bringing the p ‐band center of carbon active sites closer to the Fermi level, thereby giving rise to a new concept catalytic system of GDY/RhO x /NiO. Both the theoretical and experimental results evidenced the obvious charge redistribution and strong p‐d orbital coupling at the heterointerface, greatly enhancing the spatial charge inhomogeneity and improving the transformative electrocatalytic hydrogen evolution capability under alkaline conditions, with overpotentials of 60 and 67 mV to deliver large current densities of 500 and 1000 mA cm −2 , respectively, and robust stability at industrial‐grade current densities for 200 h. This intelligent charge regulation strategy through differential p‐d orbital coupling provides a new direction for the design of high‐performance catalysts in industrial electrocatalytic processes.