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Title: Diversity of Adsorbed Hydrogen on the TiC(001) Surface at High Coverages

Abstract

The catalyzed dissociation of molecular hydrogen on the surfaces of diverse materials is currently widely studied due to its importance in a broad range of hydrogenation reactions that convert noxious exhaust products and/or greenhouse gases into added-value greener products, such as methanol. In the search for viable replacements for expensive late-transition-metal catalysts, TiC has been increasingly investigated as a potential catalyst for H 2 dissociation. Here, we report on a combination of experiments and density functional theory calculations on the well-defined TiC(001) surface, revealing that multiple H and H 2 species are available on this substrate, with different binding configurations and adsorption energies. Here, our calculations predict an initial occupancy of H atoms on the surface C atom sites, which then enables the subsequent stabilization of H atoms on top of the surface Ti atoms. Further H 2 can be also molecularly adsorbed over Ti sites. These theoretical predictions are in full accordance with information extracted from X-ray photoemission spectroscopy and temperature-programmed desorption experiments. The experimental results show that at high coverages of hydrogen, there is a reconstruction of the TiC(001) surface, which facilitates the binding of hydrogen.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]
  1. Univ. de Barcelona, Barcelona (Spain). Dept. de Ciència de Materials i Química Física & Inst. de Química Teòrica i Computacional (IQTCUB)
  2. Univ. Central de Venezuela, Caracas (Venezuela). Facultad de Ciencias
  3. Univ. de Barcelona, Barcelona (Spain). Dept. de Ciència de Materials i Química Física & Inst. de Química Teòrica i Computacional (IQTCUB); Institució Catalana de Recerca i Estudis Avançats (ICREA), Barcelona (Spain)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1484881
Report Number(s):
BNL-209647-2018-JAAM
Journal ID: ISSN 1932-7447
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Name: Journal of Physical Chemistry. C; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Piñero, Juan José, Ramírez, Pedro J., Bromley, Stefan T., Illas, Francesc, Viñes, Francesc, and Rodriguez, José A. Diversity of Adsorbed Hydrogen on the TiC(001) Surface at High Coverages. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b07340.
Piñero, Juan José, Ramírez, Pedro J., Bromley, Stefan T., Illas, Francesc, Viñes, Francesc, & Rodriguez, José A. Diversity of Adsorbed Hydrogen on the TiC(001) Surface at High Coverages. United States. doi:10.1021/acs.jpcc.8b07340.
Piñero, Juan José, Ramírez, Pedro J., Bromley, Stefan T., Illas, Francesc, Viñes, Francesc, and Rodriguez, José A. Fri . "Diversity of Adsorbed Hydrogen on the TiC(001) Surface at High Coverages". United States. doi:10.1021/acs.jpcc.8b07340.
@article{osti_1484881,
title = {Diversity of Adsorbed Hydrogen on the TiC(001) Surface at High Coverages},
author = {Piñero, Juan José and Ramírez, Pedro J. and Bromley, Stefan T. and Illas, Francesc and Viñes, Francesc and Rodriguez, José A.},
abstractNote = {The catalyzed dissociation of molecular hydrogen on the surfaces of diverse materials is currently widely studied due to its importance in a broad range of hydrogenation reactions that convert noxious exhaust products and/or greenhouse gases into added-value greener products, such as methanol. In the search for viable replacements for expensive late-transition-metal catalysts, TiC has been increasingly investigated as a potential catalyst for H2 dissociation. Here, we report on a combination of experiments and density functional theory calculations on the well-defined TiC(001) surface, revealing that multiple H and H2 species are available on this substrate, with different binding configurations and adsorption energies. Here, our calculations predict an initial occupancy of H atoms on the surface C atom sites, which then enables the subsequent stabilization of H atoms on top of the surface Ti atoms. Further H2 can be also molecularly adsorbed over Ti sites. These theoretical predictions are in full accordance with information extracted from X-ray photoemission spectroscopy and temperature-programmed desorption experiments. The experimental results show that at high coverages of hydrogen, there is a reconstruction of the TiC(001) surface, which facilitates the binding of hydrogen.},
doi = {10.1021/acs.jpcc.8b07340},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
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