Hydrogen spillover mechanism on a Pd-doped Mg surface as revealed by ab initio density functional calculation

J Am Chem Soc. 2007 Aug 22;129(33):10201-4. doi: 10.1021/ja0722776. Epub 2007 Jul 31.

Abstract

The hydrogenation kinetics of Mg is slow, impeding its application for mobile hydrogen storage. We demonstrate by ab initio density functional theory (DFT) calculations that the reaction path can be greatly modified by adding transition metal catalysts. Contrasting with Ti doping, a Pd dopant will result in a very small activation barrier for both dissociation of molecular hydrogen and diffusion of atomic H on the Mg surface. This new computational finding supports-for the first time by ab initio simulation-the proposed hydrogen spillover mechanism for rationalizing experimentally observed fast hydrogenation kinetics for Pd-capped Mg materials.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Hydrogen / chemistry*
  • Kinetics
  • Magnesium / chemistry*
  • Models, Molecular
  • Palladium / chemistry*
  • Surface Properties
  • Thermodynamics
  • Titanium / chemistry

Substances

  • Palladium
  • Hydrogen
  • Titanium
  • Magnesium