Kinetics of H2 Adsorption at the Metal–Support Interface of Au/TiO2 Catalysts Probed by Broad Background IR Absorbance

Akbar Mahdavi-Shakib; K. B.Sravan Kumar; Todd N. Whittaker; Tianze Xie; Lars C. Grabow; Robert M. Rioux; Bert D. Chandler

doi:10.1002/anie.202013359

Kinetics of H₂ Adsorption at the Metal–Support Interface of Au/TiO₂ Catalysts Probed by Broad Background IR Absorbance

Akbar Mahdavi-Shakib, K. B.Sravan Kumar, Todd N. Whittaker, Tianze Xie, Lars C. Grabow, Robert M. Rioux, Bert D. Chandler

Research output: Contribution to journal › Article › peer-review

33 Scopus citations

Abstract

H₂ adsorption on Au catalysts is weak and reversible, making it difficult to quantitatively study. We demonstrate H₂ adsorption on Au/TiO₂ catalysts results in electron transfer to the support, inducing shifts in the FTIR background. This broad background absorbance (BBA) signal is used to quantify H₂ adsorption; adsorption equilibrium constants are comparable to volumetric adsorption measurements. H₂ adsorption kinetics measured with the BBA show a lower E_app value (23 kJ mol⁻¹) for H₂ adsorption than previously reported from proxy H/D exchange (33 kJ mol⁻¹). We also identify a previously unreported H-O-H bending vibration associated with proton adsorption on electronically distinct Ti-OH metal-support interface sites, providing new insight into the nature and dynamics of H₂ adsorption at the Au/TiO₂ interface.

Original language	English (US)
Pages (from-to)	7735-7743
Number of pages	9
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	14
DOIs	https://doi.org/10.1002/anie.202013359
State	Published - Mar 29 2021

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry

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title = "Kinetics of H2 Adsorption at the Metal–Support Interface of Au/TiO2 Catalysts Probed by Broad Background IR Absorbance",

abstract = "H2 adsorption on Au catalysts is weak and reversible, making it difficult to quantitatively study. We demonstrate H2 adsorption on Au/TiO2 catalysts results in electron transfer to the support, inducing shifts in the FTIR background. This broad background absorbance (BBA) signal is used to quantify H2 adsorption; adsorption equilibrium constants are comparable to volumetric adsorption measurements. H2 adsorption kinetics measured with the BBA show a lower Eapp value (23 kJ mol−1) for H2 adsorption than previously reported from proxy H/D exchange (33 kJ mol−1). We also identify a previously unreported H-O-H bending vibration associated with proton adsorption on electronically distinct Ti-OH metal-support interface sites, providing new insight into the nature and dynamics of H2 adsorption at the Au/TiO2 interface.",

author = "Akbar Mahdavi-Shakib and Kumar, \{K. B.Sravan\} and Whittaker, \{Todd N.\} and Tianze Xie and Grabow, \{Lars C.\} and Rioux, \{Robert M.\} and Chandler, \{Bert D.\}",

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AU - Mahdavi-Shakib, Akbar

AU - Kumar, K. B.Sravan

AU - Whittaker, Todd N.

AU - Xie, Tianze

AU - Grabow, Lars C.

AU - Rioux, Robert M.

AU - Chandler, Bert D.

PY - 2021/3/29

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N2 - H2 adsorption on Au catalysts is weak and reversible, making it difficult to quantitatively study. We demonstrate H2 adsorption on Au/TiO2 catalysts results in electron transfer to the support, inducing shifts in the FTIR background. This broad background absorbance (BBA) signal is used to quantify H2 adsorption; adsorption equilibrium constants are comparable to volumetric adsorption measurements. H2 adsorption kinetics measured with the BBA show a lower Eapp value (23 kJ mol−1) for H2 adsorption than previously reported from proxy H/D exchange (33 kJ mol−1). We also identify a previously unreported H-O-H bending vibration associated with proton adsorption on electronically distinct Ti-OH metal-support interface sites, providing new insight into the nature and dynamics of H2 adsorption at the Au/TiO2 interface.

AB - H2 adsorption on Au catalysts is weak and reversible, making it difficult to quantitatively study. We demonstrate H2 adsorption on Au/TiO2 catalysts results in electron transfer to the support, inducing shifts in the FTIR background. This broad background absorbance (BBA) signal is used to quantify H2 adsorption; adsorption equilibrium constants are comparable to volumetric adsorption measurements. H2 adsorption kinetics measured with the BBA show a lower Eapp value (23 kJ mol−1) for H2 adsorption than previously reported from proxy H/D exchange (33 kJ mol−1). We also identify a previously unreported H-O-H bending vibration associated with proton adsorption on electronically distinct Ti-OH metal-support interface sites, providing new insight into the nature and dynamics of H2 adsorption at the Au/TiO2 interface.

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Kinetics of H₂ Adsorption at the Metal–Support Interface of Au/TiO₂ Catalysts Probed by Broad Background IR Absorbance

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