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Oxidation state and local structure of Ti-based additives in the Reactive Hydride Composite 2LiBH₄ + MgH₂

ICMS

E. Deprez, Miguel A. Muñoz-Márquez, Manuel A. Roldán, C. Prestipino, F. Javier Palomares, C. Bonatto Minella, U. Bösenberg, M. Dornheim, R. Bormann, A. Fernández Journal of Physical Chemistry C 2010, Vol. 114, 3309-3317

Nowadays, the technological utilization of Reactive Hydride Composites (RHC) as hydrogen storage materials is limited by their reaction kinetics. However, addition of transition metal based additives, for instance titanium isopropoxide (Ti-iso), to the 2LiBH₄+MgH₂ system, results in a significant improvement of sorption kinetics. In this work, the evolution of chemical state and local structure of the Ti-based additive has been investigated by means of X-ray absorption (XAS) and photoemission (XPS) spectroscopy. X-ray absorption near-edge structure (XANES), as well as extended X-ray absorption fine structure (EXAFS) analysis, have been undertaken at the Ti K-edge. The measurements reveal the formation of a highly dispersed and disordered TiO2-like phase during ball milling. During first desorption reduced titanium oxide and titanium boride are formed and remain stable upon cycling. The surface analysis performed by XPS shows that the reduction processes of the Ti-based additive during first desorption is coupled to the migration of the Ti species from the surface to the bulk of the material. Several factors, related to favouring heterogeneous nucleation of MgB2 and the increase of interfacial area through grain refinement are proposed as potential driving force, among other effects, for the observed kinetic improvement.

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