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Travert A, Nakamura H, van Santen RA, et al. Hydrogen activation on Mo-based sulfide catalysts, a periodic DFT study. J Am Chem Soc. 2002;124(24):7084-95doi: 10.1021/ja011634o.
Travert, A., Nakamura, H., van Santen, R. A., Cristol, S., Paul, J. F., & Payen, E. (2002). Hydrogen activation on Mo-based sulfide catalysts, a periodic DFT study. Journal of the American Chemical Society, 124(24), 7084-95. https://doi.org/10.1021/ja011634o
Travert, Arnaud, et al. "Hydrogen activation on Mo-based sulfide catalysts, a periodic DFT study." Journal of the American Chemical Society vol. 124,24 (2002): 7084-95. doi: https://doi.org/10.1021/ja011634o
Travert A, Nakamura H, van Santen RA, Cristol S, Paul JF, Payen E. Hydrogen activation on Mo-based sulfide catalysts, a periodic DFT study. J Am Chem Soc. 2002 Jun 19;124(24):7084-95. doi: 10.1021/ja011634o. PMID: 12059233.
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J Am Chem Soc. 2002 Jun 19;124(24):7084-95. doi: 10.1021/ja011634o.

Hydrogen activation on Mo-based sulfide catalysts, a periodic DFT study.

Journal of the American Chemical Society

Arnaud Travert, Hiroyuki Nakamura, Rutger A van Santen, Sylvain Cristol, Jean-François Paul, Edmond Payen

Affiliations

  1. Schuit Institute of Catalysis, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands. [email protected]

PMID: 12059233 DOI: 10.1021/ja011634o

Abstract

Hydrogen adsorption on Mo[bond]S, Co[bond]Mo[bond]S, and Ni[bond]Mo[bond]S (10 1 macro 0) surfaces has been modeled by means of periodic DFT calculations taking into account the gaseous surrounding of these catalysts in working conditions. On the stable Mo[bond]S surface, only six-fold coordinated Mo cations are present, whereas substitution by Co or Ni leads to the creation of stable coordinatively unsaturated sites. On the stable MoS(2) surface, hydrogen dissociation is always endothermic and presents a high activation barrier. On Co[bond]Mo[bond]S surfaces, the ability to dissociate H(2) depends on the nature of the metal atom and the sulfur coordination environment. As an adsorption center, Co strongly favors molecular hydrogen activation as compared to the Mo atoms. Co also increases the ability of its sulfur atom ligands to bind hydrogen. Investigation of surface acidity using ammonia as a probe molecule confirms the crucial role of sulfur basicity on hydrogen activation on these surfaces. As a result, Co[bond]Mo[bond]S surfaces present Co[bond]S sites for which the dissociation of hydrogen is exothermic and weakly activated. On Ni[bond]Mo[bond]S surfaces, Ni[bond]S pairs are not stable and do not provide for an efficient way for hydrogen activation. These theoretical results are in good agreement with recent experimental studies of H(2)[bond]D(2) exchange reactions.

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