TY - JOUR
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
N1 - Funding Information:
This material is based upon work supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Advanced Manufacturing Office Award Number DE-EE0007897 awarded to the REMADE Institute, a division of Sustainable Manufacturing Innovation Alliance Corp. Training was provided by the Computational Materials Education and Training (CoMET) NSF Research Traineeship (Grant No. DGE-1449785). Computational resources were provided through the Extreme Science and Engineering Discovery Environment (XSEDE) supported by the National Science Foundation (Grant No. ACI-1548562).
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
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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U2 - 10.1021/acs.jpcc.2c01670
DO - 10.1021/acs.jpcc.2c01670
M3 - Article
AN - SCOPUS:85129243680
SN - 1932-7447
VL - 126
SP - 7482
EP - 7491
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 17
ER -