Abstract
Metal d-band configuration is decisive to the interaction of metals with reactants and intermediates, therefore often governs the catalytic activity. Herein, we for the first time demonstrate a family of alkali tungsten bronzes (MxWO3, M = Na, K, Rb, Cs and 0<x<1) for efficient hydrogen evolution reaction (HER) by modulating the W-d band configuration. Experimental and theoretical investigations on the newly-reported alkali tungsten bronzes reveal a linear relationship between the W-5d band center and the HER activity. Guided by this, the introduction of sodium ions endows NaxWO3 with optimized electronic structure and W-d band configuration, leading to not only superior charge-transfer ability but also promoted H2O adsorption/dissociation kinetics and moderate hydrogen adsorption energy for wide-pH HER. As a result, NaxWO3 exhibits Pt-like activity in a wide-pH range, delivering an overpotential as low as 37, 48 and 226 mV at 10 mA cm−2 in acid, alkaline and neutral seawater, respectively. This work provides the first insight into the role of alkali metal ions in tungsten bronzes towards HER, which thus is expected to open up a new class of non-precious metal-based electrocatalysts for the HER and other energy storage and conversion reactions.
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