Modulating the electronic structure of platinum (Pt) through a support is an important strategy for enhancing its electrocatalytic properties. In this work, to explore the impact of support electronegativity on Pt's catalytic activity for hydrogen evolution, we chose diverse metals with varying electronegativities that are stable in acidic solutions, such as titanium (Ti), molybdenum (Mo), and tungsten (W), as supports. Ti is the optimal support according to density functional theory (DFT) calculations. As expected, the Pt@Ti catalyst demonstrated remarkable efficiency in the hydrogen evolution reaction (HER), displaying a minimal overpotential of 13 mV at -10 mA cm-2, a Tafel slope of 34.5 mV dec-1, and sustained durability over 110 h in a 0.5 M H2SO4 solution. To unravel the metal-support interaction (MSI) between Pt and Ti, a comprehensive exploration encompassing both experimental investigations and DFT calculations was undertaken. The results elucidate that the outstanding HER performance of Pt@Ti stems from robust synergies forged between Pt and Ti atoms within the Ti support. This work not only furnishes a technique for producing electrocatalysts with superior efficiency and stability but also streamlines the process of choosing the most appropriate metal support. Moreover, it enhances comprehension of the interaction between Pt and the metal support.
Keywords: Electronegativity; Hydrogen evolution reaction; Metal-support interaction; Support.
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