Abstract
Titanium dioxide, with excellent stability, high catalytic activity and abundant reserves, is an ideal substitute for noble metals in hydrogen reaction reactions (HER). However, the strong *H adsorption makes it only a substrate. Tuning metal-oxygen covalency can effectively optimize the adsorption energy. Herein, Ru-modified TiO2 with different phases (rutile, anatase and their mixed-phase) is synthesized, where metal-oxygen covalency and phase transition synergistically boost HER. The target m-Ru@TiO2-x exhibits high HER activity under large current density in wide pH, requiring low overpotential of 87/284 mV (acidic), and 47/366 mV (alkaline) to deliver 10 and 1000 mA·cm−2, respectively, superior to benchmark Pt/C. Theoretical calculation shows that Ru incorporation and mixed rutile-anatase endow m-Ru@TiO2-x with a more negative O p band and decreased overlap between Ti d and O p states, ultimately expediting the desorption of hydrogen during HER. This work enlightens an efficient pathway for tuning the metal-oxygen covalency in HER catalysts.
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