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The role of surface hydroxyls in the entropy-driven adsorption and spillover of H2 on Au/TiO2 catalysts
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The role of surface hydroxyls in the entropy-driven adsorption and spillover of H2 on Au/TiO2 catalysts
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Journal Article
The role of surface hydroxyls in the entropy-driven adsorption and spillover of H2 on Au/TiO2 catalysts
2023
Overview
Hydrogen spillover involves the migration of H atom equivalents from metal nanoparticles to a support. While well documented, H spillover is poorly understood and largely unquantified. Here we measure weak, reversible H
2
adsorption on Au/TiO
2
catalysts, and extract the surface concentration of spilled-over hydrogen. The spillover species (H*) is best described as a loosely coupled proton/electron pair distributed across the titania surface hydroxyls. In stark contrast to traditional gas adsorption systems, H* adsorption increases with temperature. This unexpected adsorption behaviour has two origins. First, entropically favourable adsorption results from high proton mobility and configurational surface entropy. Second, the number of spillover sites increases with temperature, due to increasing hydroxyl acid–base equilibrium constants. Increased H* adsorption correlates with the associated changes in titania surface zwitterion concentration. This study provides a quantitative assessment of how hydroxyl surface chemistry impacts spillover thermodynamics, and contributes to the general understanding of spillover phenomena.
Spillover phenomena are crucial in heterogeneous catalysis, yet remain elusive to quantitative characterization. Here the authors measure the surface concentration of hydrogen spilling-over onto TiO
2
using Au/TiO
2
catalysts and explain the underlying factors governing the process.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Springer Nature
Subject
