Site-Dependent Activity of Atomic Ti Catalysts in Al-Based Hydrogen Storage Materials.

Doping catalytically inactive materials with dispersed atoms of an active species is a promising route toward realizing ultradilute binary catalyst systems. Beyond catalysis, strategically placed metal atoms can accelerate a wide range of solid-state reactions, particularly in hydrogen storage proce...

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Published in:Journal of the American Chemical Society Vol. 134; no. 25; pp. 10381 - 10385
Main Authors: Al-Mahboob, Abdullah, Muller, Erik, Karim, Altaf, Muckerman, James T., Ciobanu, Cristian V., Sutter, Peter
Format: Article
Published: American Chemical Society 6/27/2012
Subjects:
Online Access:View this record in EBSCOhost
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        10.1021/ja304203y
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        atl: Site-Dependent Activity of Atomic Ti Catalysts in Al-Based Hydrogen Storage Materials.
      aug:
        au:
          Al-Mahboob, Abdullah
          Muller, Erik
          Karim, Altaf
          Muckerman, James T.
          Ciobanu, Cristian V.
          Sutter, Peter
        affil:
          Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States
          Department of Chemistry, Brookhaven National Laboratory, Upton, New York 11973, United States
          Department of Mechanical Engineering, Materials Science Program, Colorado School of Mines, Golden, Colorado 80401, United States
      su:
        Titanium catalyst activity
        Hydrogen storage
        Aluminum
        Hydrogenation
        Doping agents (Chemistry)
        Dissociation (Chemistry)
      sug:
        subj:
          Titanium catalyst activity
          Hydrogen storage
          Aluminum
          Hydrogenation
          Doping agents (Chemistry)
          Dissociation (Chemistry)
      ab: Doping catalytically inactive materials with dispersed atoms of an active species is a promising route toward realizing ultradilute binary catalyst systems. Beyond catalysis, strategically placed metal atoms can accelerate a wide range of solid-state reactions, particularly in hydrogen storage processes. Here we analyze the role of atomic Ti catalysts in the hydrogenation of Al-based hydrogen storage materials. We show that Ti atoms near the Al surface activate gas-phase H a key step toward hydrogenation. By controlling the placement of Ti, we have found that the overall reaction, comprising H dissociation and H spillover onto the Al surface, is governed by a pronounced trade-off between lowering of the H dissociation barrier and trapping of the products near the active site, with a sharp maximum in the overall activity for Ti in the subsurface layer. Our findings demonstrate the importance of controlling the placement of the active species in optimizing the activity of dilute binary systems.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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