Confinement of MgH2 nanoclusters within nanoporous aerogel scaffold materials.

Nanoparticles of magnesium hydride were embedded in nanoporous carbon aerogel scaffold materials in order to explore the kinetic properties of hydrogen uptake and release. A new modified procedure for the synthesis of magnesium hydride nanoparticles is presented. The procedure makes use of monoliths (approximately 0.4 cm(3)) of two distinct types of nanoporous resorcinol-formaldehyde carbon aerogels loaded with dibutylmagnesium, MgBu(2). Excess MgBu(2) was removed mechanically, and the increase in mass was used as a measure of the amount of embedded MgH(2). Energy-dispersive spectrometry revealed that MgH(2) was uniformly distributed within the aerogel material. In situ synchrotron radiation powder X-ray diffraction showed that MgBu(2) transformed directly to MgH(2) at T approximately 137 degrees C and p(H(2)) = 50 bar. Two distinct aerogel samples, denoted X1 and X2, with pore volumes of 1.27 and 0.65 mL/g and average pore sizes of 22 and 7 nm, respectively, were selected. In these samples, the uptake of magnesium hydride was found to be proportional to the pore volume, and aerogels X1 and X2 incorporated 18.2 and 10.0 wt % of MgH(2), respectively. For the two samples, the volumetric MgH(2) uptake was similar, approximately 12 vol %. The hydrogen storage properties of nanoconfined MgH(2) were studied by Sieverts' measurements and thermal desorption spectroscopy, which clearly demonstrated that the dehydrogenation kinetics of the confined hydride depends on the pore size distribution of the scaffold material; that is, smaller pores mediated faster desorption rates possibly due to a size reduction of the confined magnesium hydride.

[1]  Ping Liu,et al.  Fabrication and hydrogen sorption behaviour of nanoparticulate MgH2 incorporated in a porous carbon host , 2009, Nanotechnology.

[2]  Ping Liu,et al.  The synthesis and hydrogen storage properties of a MgH2 incorporated carbon aerogel scaffold , 2009, Nanotechnology.

[3]  G. Lu,et al.  Magnesium-based materials for hydrogen storage: Recent advances and future perspectives , 2008 .

[4]  M. Dresselhaus,et al.  Impact of nanostructuring on the enthalpy of formation of metal hydrides , 2008 .

[5]  John J. Vajo,et al.  Enhanced Hydrogen Storage Kinetics of LiBH4 in Nanoporous Carbon Scaffolds , 2008 .

[6]  Zhonghua Zhu,et al.  Hydrogen diffusion and effect of grain size on hydrogenation kinetics in magnesium hydrides , 2008 .

[7]  G. Olson,et al.  Thermodynamic destabilization and reaction kinetics in light metal hydride systems , 2007 .

[8]  John W. Geus,et al.  The Preparation of Carbon-Supported Magnesium Nanoparticles using Melt Infiltration , 2007 .

[9]  Ulrich Eberle,et al.  Hydrogen storage: the remaining scientific and technological challenges. , 2007, Physical Chemistry, Chemical Physics - PCCP.

[10]  Gang Chen,et al.  Size effects on the hydrogen storage properties of nanostructured metal hydrides: A review , 2007 .

[11]  A. Züttel,et al.  Complex hydrides for hydrogen storage. , 2007, Chemical reviews.

[12]  Jun Li,et al.  Studies on preparation and performances of carbon aerogel electrodes for the application of supercapacitor , 2006 .

[13]  M. Dornheim,et al.  Tailoring Hydrogen Storage Materials Towards Application , 2006 .

[14]  J. H. van Lenthe,et al.  Hydrogen storage in magnesium clusters: quantum chemical study. , 2005, Journal of the American Chemical Society.

[15]  Siegmar Roth,et al.  Hydrogen adsorption in different carbon nanostructures , 2005 .

[16]  B. D. Kay,et al.  Nanoscaffold mediates hydrogen release and the reactivity of ammonia borane. , 2005, Angewandte Chemie.

[17]  A. V. van Duin,et al.  ReaxFF(MgH) reactive force field for magnesium hydride systems. , 2005, The journal of physical chemistry. A.

[18]  J. J. Liang Theoretical insight on tailoring energetics of Mg hydrogen absorption/desorption through nano-engineering , 2005 .

[19]  M. Nielsen,et al.  Interaction of hydrogen with an Mg–Al alloy , 2005 .

[20]  A. Lu,et al.  Hard-Templating Pathway To Create Mesoporous Magnesium Oxide , 2004 .

[21]  W. Grochala,et al.  Thermal Decomposition of the Non‐Interstitial Hydrides for the Storage and Production of Hydrogen , 2004 .

[22]  Miroslav Haluska,et al.  Thermal desorption spectroscopy as a quantitative tool to determine the hydrogen content in solids , 2003 .

[23]  J. A. Ritter,et al.  Implementing a hydrogen economy , 2003 .

[24]  H. Aoki,et al.  TED-AJ03-145 NUMERICAL ANALYSIS OF ABSORBING AND DESORBING MECHANISM FOR THE METAL HYDRIDE BY HOMOGENIZATION METHOD , 2003 .

[25]  James A. Ritter,et al.  Preparation and Properties of Resorcinol–Formaldehyde Organic and Carbon Gels , 2003 .

[26]  A. Züttel,et al.  Hydrogen-storage materials for mobile applications , 2001, Nature.

[27]  L. Berlouis,et al.  Thermal analysis investigation of hydriding properties of nanocrystalline Mg–Ni- and Mg–Fe-based alloys prepared by high-energy ball milling , 2001 .

[28]  A. Załuska,et al.  Nanocrystalline magnesium for hydrogen storage , 1999 .

[29]  M. Hirscher,et al.  Influence of the microstructure on the desorption kinetics of single- and multiphase LaNiFe alloys , 1998 .

[30]  A. Załuska,et al.  Nanocrystalline metal hydrides , 1997 .

[31]  R. Birringer,et al.  On the room-temperature grain growth in nanocrystalline copper , 1994 .

[32]  R. Birringer,et al.  Hydrogen in amorphous and nanocrystalline metals , 1988 .

[33]  A. Pedersen,et al.  Elements of hydride formation mechanisms in nearly spherical magnesium powder particles , 1987 .

[34]  A. Pedersen,et al.  Hydrogen sorption performance of pure magnesium during continued cycling , 1983 .

[35]  A. Pedersen,et al.  Formation and decomposition of magnesium hydride , 1983 .

[36]  J. Boer,et al.  Studies on pore systems in catalysts: VII. Description of the pore dimensions of carbon blacks by the t method , 1965 .

[37]  E. Barrett,et al.  The Determination of Pore Volume and Area Distributions in Porous Substances. II. Comparison between Nitrogen Isotherm and Mercury Porosimeter Methods , 1951 .

[38]  E. Barrett,et al.  (CONTRIBUTION FROM THE MULTIPLE FELLOWSHIP OF BAUGH AND SONS COMPANY, MELLOX INSTITUTE) The Determination of Pore Volume and Area Distributions in Porous Substances. I. Computations from Nitrogen Isotherms , 1951 .

[39]  F. Tompkins Physical adsorption on non-uniform surfaces , 1950 .

[40]  E. Teller,et al.  ADSORPTION OF GASES IN MULTIMOLECULAR LAYERS , 1938 .