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    Hydrogen absorption kinetics of the transition-metal-chloride-enhanced NaAlH4 system

    Access Status
    Fulltext not available
    Authors
    Pitt, M.
    Vullum, P.
    Sørby, M.
    Emerich, H.
    Paskevicius, Mark
    Buckley, Craig
    Walmsley, J.
    Holmestad, R.
    Hauback, B.
    Date
    2012
    Type
    Journal Article
    
    Metadata
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    Citation
    Pitt, Mark P. and Vullum, Per E. and Sørby, Magnus H. and Emerich, Hermann and Paskevicius, Mark and Buckley, Craig E. and Walmsley, John C. and Holmestad, Randi and Hauback, Bjorn C. 2012. Hydrogen absorption kinetics of the transition-metal-chloride-enhanced NaAlH4 system. The Journal of Physical Chemistry C. 116 (27): pp. 14205-14217.
    Source Title
    The Journal of Physical Chemistry C
    DOI
    10.1021/jp3042654
    ISSN
    1932-7447
    URI
    http://hdl.handle.net/20.500.11937/32256
    Collection
    • Curtin Research Publications
    Abstract

    This study elucidates the role of transition metal (TM) additives in enhancing hydrogen (H) reversibility and hydrogenation kinetics for the NaAlH4 system. The isothermal hydrogen absorption kinetics of the planetary milled (PM) NaAlH4 + xTMCln (TM row 1 = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu; row 2 = Zn, Y, Zr, Nb, Mo, Ru, Rh Pd; row 3 = Pt; 2 < n < 5) and cryo-milled (CM) NaAlH4 + xTMCln (TM row 1 = Ti, V, Cr, Fe, Co, Ni, Cu; 2 < n < 3) systems have been measured at 140 °C and 150 bar system pressure. The variation in hydrogenation kinetics across the TM series for NaAlH4 + xTMCln is strongly dependent on the TM species and additive level, milling technique, and the type, structure, and morphological arrangement of nanoscopic Al1−xTMx phases that are embedded on the NaAlH4 surface. In the most interesting case, the surface-embedded Al1−xTix phases in the TiCl3-enhanced NaAlH4 system perform a dual catalytic function, where the outer Al1−xTix surface performs dissociation/recombination of molecular H2 and the inner Al1−xTix surface allows the distortion of a minor number of Al−H bonds from AlH4 − tetrahedra in the vicinity of the subsurface Al1−xTix/NaAlH4 interface. The density of Ti atoms in the subsurface interface (which is Al:Ti composition- and H cycling temperature-dependent) shows the strongest effects on hydrogenation kinetics.

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