Hydrogen Activation and Spillover on Anatase TiO2-Supported Ag Single-Atom Catalysts

Jeremy Hu; Eun Mi Kim; Michael J. Janik; Konstantinos Alexopoulos

doi:10.1021/acs.jpcc.2c01670

Hydrogen Activation and Spillover on Anatase TiO₂-Supported Ag Single-Atom Catalysts

Jeremy Hu, Eun Mi Kim, Michael J. Janik, Konstantinos Alexopoulos

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

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Abstract

Density functional theory (DFT) was used to examine the mechanisms of hydrogen activation and spillover on anatase TiO₂-supported Ag single-atom catalysts. Stable structures of Ag were proposed on the (001) facet, considered a more catalytically active surface, and (101), a more stable facet. Surface oxygen vacancies (O_vac) were more favorably formed in the presence of Ag single atoms, reducing the energy of O_vacformation by 0.5 eV on (001) and 0.9 eV on (101). Ag single atoms adsorbed on TiO₂(001) and (101) surfaces promote H₂dissociative adsorption through a heterolytic mechanism, with an average activation barrier of 0.26 eV. Finally, reaction energies were calculated that corroborate experimental results of continuous hydrogen spillover from Ag to the TiO₂support.

Original language	English (US)
Pages (from-to)	7482-7491
Number of pages	10
Journal	Journal of Physical Chemistry C
Volume	126
Issue number	17
DOIs	https://doi.org/10.1021/acs.jpcc.2c01670
State	Published - May 5 2022

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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title = "Hydrogen Activation and Spillover on Anatase TiO2-Supported Ag Single-Atom Catalysts",

abstract = "Density functional theory (DFT) was used to examine the mechanisms of hydrogen activation and spillover on anatase TiO2-supported Ag single-atom catalysts. Stable structures of Ag were proposed on the (001) facet, considered a more catalytically active surface, and (101), a more stable facet. Surface oxygen vacancies (Ovac) were more favorably formed in the presence of Ag single atoms, reducing the energy of Ovacformation by 0.5 eV on (001) and 0.9 eV on (101). Ag single atoms adsorbed on TiO2(001) and (101) surfaces promote H2dissociative adsorption through a heterolytic mechanism, with an average activation barrier of 0.26 eV. Finally, reaction energies were calculated that corroborate experimental results of continuous hydrogen spillover from Ag to the TiO2support.",

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T1 - Hydrogen Activation and Spillover on Anatase TiO2-Supported Ag Single-Atom Catalysts

AU - Hu, Jeremy

AU - Kim, Eun Mi

AU - Janik, Michael J.

AU - Alexopoulos, Konstantinos

PY - 2022/5/5

Y1 - 2022/5/5

N2 - Density functional theory (DFT) was used to examine the mechanisms of hydrogen activation and spillover on anatase TiO2-supported Ag single-atom catalysts. Stable structures of Ag were proposed on the (001) facet, considered a more catalytically active surface, and (101), a more stable facet. Surface oxygen vacancies (Ovac) were more favorably formed in the presence of Ag single atoms, reducing the energy of Ovacformation by 0.5 eV on (001) and 0.9 eV on (101). Ag single atoms adsorbed on TiO2(001) and (101) surfaces promote H2dissociative adsorption through a heterolytic mechanism, with an average activation barrier of 0.26 eV. Finally, reaction energies were calculated that corroborate experimental results of continuous hydrogen spillover from Ag to the TiO2support.

AB - Density functional theory (DFT) was used to examine the mechanisms of hydrogen activation and spillover on anatase TiO2-supported Ag single-atom catalysts. Stable structures of Ag were proposed on the (001) facet, considered a more catalytically active surface, and (101), a more stable facet. Surface oxygen vacancies (Ovac) were more favorably formed in the presence of Ag single atoms, reducing the energy of Ovacformation by 0.5 eV on (001) and 0.9 eV on (101). Ag single atoms adsorbed on TiO2(001) and (101) surfaces promote H2dissociative adsorption through a heterolytic mechanism, with an average activation barrier of 0.26 eV. Finally, reaction energies were calculated that corroborate experimental results of continuous hydrogen spillover from Ag to the TiO2support.

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Hydrogen Activation and Spillover on Anatase TiO₂-Supported Ag Single-Atom Catalysts

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