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Quaternary Ammonium Borohydride Adsorption in Mesoporous Silicate MCM-48

Published online by Cambridge University Press:  01 February 2011

Michael Joseph Wolverton ,
Luc L. Daemen  and
Monika A. Hartl
Michael Joseph Wolverton
Affiliation:
[email protected]
Luc L. Daemen
Affiliation:
[email protected], LANL, LANSCE, Los Alamos, United States
Monika A. Hartl
Affiliation:
[email protected], LANL, LANSCE, Los Alamos, United States
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Abstract

Inorganic borohydrides have a high gravimetric hydrogen density but release H2 only under energetically unfavorable conditions. Surface chemistry may help in lowering thermodynamic barriers, but inclusion of inorganic borohydrides in porous silica materials has proved hitherto difficult or impossible. We show that borohydrides with a large organic cation are readily adsorbed inside mesoporous silicates, particularly after surface treatment. Thermal analysis reveals that the decomposition thermodynamics of tetraalkylammonium borohydrides are substantially affected by inclusion in MCM-48. Inelastic neutron scattering (INS) data show that the compounds adsorb on the silica surface. Evidence of pore loading is supplemented by DSC/TGA, XRD, FTIR, and BET isotherm measurements. Mass spectrometry shows significant hydrogen release at lower temperature from adsorbed borohydrides in comparison with the bulk borohydrides. INS data from partially decomposed samples indicates that the decomposition of the cation and anion is likely simultaneous. These data confirm the formation of Si-H bonds on the silica surface upon decomposition of adsorbed tetramethylammonium borohydride.

Keywords

adsorptionneutron scatteringsurface chemistry
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1262: Symposium V/W – In-Situ and operando Probing of Energy Materials at Multiscale Down to Single Atomic Couumn-The Powerof X-Rays, Neutons and Electrons Microscopy , 2010 , 1262-W03-03
Copyright
Copyright © Materials Research Society 2010

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