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Electrocatalytic Hydrogen Evolution at Full Atomic Utilization over ITO-Supported Sub-nano-Pt Clusters: High,
Simran Kumari1, Tsugunosuke Masubuchi2, Henry S White2
1Chemical and Biomolecular Engineering Department, University of California, Los Angeles, California 90095, United States.
Abstract:
A combination of density functional theory (DFT) and experiments with atomically size-selected Pt clusters deposited on indium-tin oxide (ITO) electrodes was used to examine the effects of applied potential and Pt size on the electrocatalytic activity of Pt (n = 1, 4, 7, and 8) for the hydrogen evolution reaction (HER). Activity is found to be negligible for isolated Pt atoms on ITO, increasing rapidly with Pt size such that Pt7/ITO and Pt8/ITO have roughly double the activity per Pt atom compared to atoms in the surface layer of polycrystalline Pt. Both the DFT and experiment find that hydrogen under-potential deposition (Hupd) results in Pt/ITO (n = 4, 7, and 8) adsorbing ∼2H atoms/Pt atom at the HER threshold potential, equal to ca. double the Hupd observed for Pt bulk or nanoparticles. The cluster catalysts under electrocatalytic conditions are hence best described as a Pt hydride compound, significantly departing from a metallic Pt cluster. The exception is Pt1/ITO, where H adsorption at the HER threshold potential is energetically unfavorable. The theory combines global optimization with grand canonical approaches for the influence of potential, uncovering the fact that several metastable structures contribute to the HER, changing with the applied potential. It is hence critical to include reactions of the ensemble of energetically accessible PtH/ITO structures to correctly predict the activity vs Pt size and applied potential. For the small clusters, spillover of Hads from the clusters to the ITO support is significant, resulting in a competing channel for loss of Hads, particularly at slow potential scan rates.
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