Abstract

Directly harvesting hydrogen from water represents a green solution toward low-cost, high-efficiency, and sustainable electrochemical energy transfer and storage. Herein, a unique approach to allow maximization of the intrinsic activity and hydrogen adsorption/desorption kinetics with engineering a lattice of rhodium (Rh) for an aqueous zinc-CO2 system is reported. The enlarged Rh–Rh bonding and lattice relaxation of Rh species cause improvement of the adsorption/desorption kinetics of H*, which can directly affect the hydrogen evolution reaction (HER). An ultralow overpotential of 6.8 mV is achieved at a current density of 10 mA cm–2 from the permanent lattice relaxed Rh under acidic conditions. In a practical application in the aqueous zinc-CO2 system, its stable hydrogen generation performance is better than that of the benchmark platinum/carbon system. This work might open opportunities for the design and engineering of electrocatalysts for high-efficiency conversion from electric energy to hydrogen energy.

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