Hydrogen storage in mesoporous titanium oxide-alkali fulleride composites.
ABSTRACT Mesoporous titanium oxide-alkali fulleride composites were synthesized and characterized by X-ray diffraction, nitrogen adsorption, Raman spectroscopy, and elemental analysis. The hydrogen sorption properties of these composites were investigated at 77 K, room temperature, and 200 degrees C. A maximum overall volumetric uptake of 27.35 kg/m(3) was obtained for the lithium fulleride composite at 77 K and 100 atm, compared with 25.48 kg/m(3) for the pristine unreduced material under the same conditions. This value was less than those previously reported for bis(toluene)titanium- and bis(benzene)vanadium-reduced materials (40.46 and 33.42 kg/m(3), respectively) and also less than those found for the fulleride-free Li- and Na-reduced materials in this study (28.10 and 28.19 kg/m(3), respectively). At room temperature and 100 atm, the maximum gravimetric storage and adsorption values of fulleride-impregnated composites were 0.99 and 0.11 wt %, respectively, while the corresponding amounts for unreduced material were 0.94 and 0.10 wt %. At 200 degrees C and 100 atm, the maximum gravimetric storage and adsorption capacities of fulleride composites were less than those of the unreduced material, which were 0.62 and 0.06 wt %, respectively. Thus, inclusion of fulleride units in the pores lowered the overall gravimetric and volumetric storage relative to the fulleride-free Na- and Li-reduced counterparts. Like other reduced composites studied in our group, the enthalpies of the reduced composites showed an unusual increasing trend with surface coverage, with the greatest value (6.55 kJ/mol) measured for the Na-reduced fulleride composite. This suggests that the reduced titanium oxide surface provides the majority of the binding sites in these materials.
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ABSTRACT: Hydrogen adsorption and storage using solid-state materials is an area of much current research interest, and one of the major stumbling blocks in realizing the hydrogen economy. However, no material yet researched comes close to reaching the DOE 2015 targets of 9 wt% and 80 kg m−3 at this time. To increase the physisorption capacities of these materials, the heats of adsorption must be increased to ∼20 kJ mol−1. This can be accomplished by optimizing the material structure, creating more active species on the surface, or improving the interaction of the surface with hydrogen. The main focus of this progress report are recent advances in physisorption materials exhibiting higher heats of adsorption and better hydrogen adsorption at room temperature based on exploiting the Kubas model for hydrogen binding: (η2-H2)–metal interaction. Both computational approaches and synthetic achievements will be discussed. Materials exploiting the Kubas interaction represent a median on the continuum between metal hydrides and physisorption materials, and are becoming increasingly important as researchers learn more about their applications to hydrogen storage problems.Advanced Materials 05/2009; 21(18):1787 - 1800. · 14.83 Impact Factor
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ABSTRACT: Nitrogen-doped (1.2–4.5wt%) carbon xerogels were synthesized from carbonization of resorcinol-formaldehyde polymer in an ammonia atmosphere at various temperatures. The textural properties and the chemical nature of nitrogen in the nitrogen-doped carbon xerogels were analyzed by Ar adsorption/desorption isotherms and X-ray photoelectron spectroscopy, respectively. The maximum hydrogen uptakes were measured to be 3.2wt% at −196°C and 0.28wt% at 35°C. Hydrogen adsorption had a stronger correlation with specific surface area than nitrogen content at the low temperature of −196°C. At the higher temperature of 35°C, optimal nitrogen doping enhanced hydrogen adsorption by electronic modification of carbon in agreement with previous theoretical predictions.Carbon. 01/2009; 47(4):1171-1180.