Determination of Structure and Phase Transition of Light Element Nanocomposites in Mesoporous Silica: Case study of NHBH in MCM-41.

Nanocomposition of molecular crystal ammonia borane (AB) by embedding it in mesoporous silica leads to a remarkable enhancement of the hydrogen storage properties. To investigate the nature of a nanophase AB, we used atomic pair distribution function (PDF) analysis of synchrotron X-ray powder diffra...

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Published in:Journal of the American Chemical Society Vol. 131; no. 38; pp. 13749 - 13756
Main Authors: Hyunjeong Kim, Karkamkar, Abhi, Autrey, Tom, Chupas, Peter, Proffen, Thomas
Format: Case Study
Published: American Chemical Society 9/30/2009
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Online Access:View this record in EBSCOhost
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        atl: Determination of Structure and Phase Transition of Light Element Nanocomposites in Mesoporous Silica: Case study of NHBH in MCM-41.
      aug:
        au:
          Hyunjeong Kim
          Karkamkar, Abhi
          Autrey, Tom
          Chupas, Peter
          Proffen, Thomas
        affil:
          Lujan Neutron Scattering Center, Los Alamos National Laboratory, Los Alamos, New Mexico 87545
          Pacific Northwest National Laboratory, Richland, Washington 99352
          Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439
      su:
        Molecular crystals
        Boranes
        Optical diffraction
        Mesoporous materials
        Nanostructured materials
      sug:
        subj:
          Molecular crystals
          Boranes
          Optical diffraction
          Mesoporous materials
          Nanostructured materials
      ab: Nanocomposition of molecular crystal ammonia borane (AB) by embedding it in mesoporous silica leads to a remarkable enhancement of the hydrogen storage properties. To investigate the nature of a nanophase AB, we used atomic pair distribution function (PDF) analysis of synchrotron X-ray powder diffraction data to follow the structural evolution of AB embedded within MCM-41 at temperatures ranging from 80 to 300 K. We found that the nanophase AB residing within the mesoporous scaffold does not undergo the structural phase transition at 225 K that was observed in the neat molecular crystal. Rather, it stays in the tetragonal phase over a wide temperature range of 110 to 240 K and starts to lose structural correlation above 240 K. This finding strongly suggests that nanoconfinement of AB within mesoporous scaffolds stabilizes the high-temperature disordered tetragonal phase at a much lower temperature. PDF analyses of composite materials composed of excess AB (i.e., AB:MCM-41 > 1:1) indicates that the excess AB forms aggregates outside the mesoporous scaffold and that these aggregates have structural properties similar to neat AB, that is, the orthorhombic-to-tetragonal structural phase transition is observed at 225 K upon warming. These results may provide important insight into the mechanism behind the enhanced hydrogen storage properties of this system.
      pubtype: Academic Journal
      doctype: Case Study
      src: R
    language: English
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