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

Journal Article · · Journal of Physical Chemistry. C
 [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.
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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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1484881
Report Number(s):
BNL-209647-2018-JAAM
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 49 Vol. 122; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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