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Structure–Activity Relationships of Nickel–Hexaaluminates in Reforming Reactions Part II: Activity and Stability of Nanostructured Nickel–Hexaaluminate-Based Catalysts in the Dry Reforming of Methane

Authors

  • Thomas Roussière,

    1. R&D Solutions hte AG, the high throughput experimentation company Kurpfalzring 104, 69123 Heidelberg (Germany), Fax: (+49) 06221-749-7137
    2. Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology, Engesserstr. 20, 76131 Karlsruhe (Germany), Fax: (+49) 07216-084-4805
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  • Linus Schulz,

    1. Catalysis Research Center, Department Chemie, Technische Universität München, Lichtenbergstr.4, 85748 Garching (Germany), Fax: (+49) 089-28-913-544
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  • Korwin M. Schelkle,

    1. Organisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 270,69120 Heidelberg (Germany), Fax: (+49) 06221-544-885
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  • Guido Wasserschaff,

    1. R&D Solutions hte AG, the high throughput experimentation company Kurpfalzring 104, 69123 Heidelberg (Germany), Fax: (+49) 06221-749-7137
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  • Dr. Andrian Milanov,

    1. GCC/PG, BASF SE, Carl-Bosch-Straße 38, 67038 Ludwigshafen (Germany), Fax: (+49) 0621-606-679-354
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  • Dr. Ekkehard Schwab,

    1. GCC/PG, BASF SE, Carl-Bosch-Straße 38, 67038 Ludwigshafen (Germany), Fax: (+49) 0621-606-679-354
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  • Prof. Dr. Olaf Deutschmann,

    1. Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology, Engesserstr. 20, 76131 Karlsruhe (Germany), Fax: (+49) 07216-084-4805
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  • Dr. Andreas Jentys,

    1. Catalysis Research Center, Department Chemie, Technische Universität München, Lichtenbergstr.4, 85748 Garching (Germany), Fax: (+49) 089-28-913-544
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  • Prof. Dr. Johannes Lercher,

    1. Catalysis Research Center, Department Chemie, Technische Universität München, Lichtenbergstr.4, 85748 Garching (Germany), Fax: (+49) 089-28-913-544
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  • Dr. Stephan A. Schunk

    Corresponding author
    1. R&D Solutions hte AG, the high throughput experimentation company Kurpfalzring 104, 69123 Heidelberg (Germany), Fax: (+49) 06221-749-7137
    • R&D Solutions hte AG, the high throughput experimentation company Kurpfalzring 104, 69123 Heidelberg (Germany), Fax: (+49) 06221-749-7137===

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Abstract

Ni–hexaaluminates exhibiting a high magnetoplumbite or β“-alumina phase content (>80 wt %) and high specific surface areas (10–30 m2 g−1) were investigated under dry reforming conditions. Ni content and choice of mirror plane cation are the key factors controlling the structure–property relationship in the dry reforming reaction of CH4. The Ni content is favorably kept below a threshold of y=0.25 in ANiyAl12-yO19−δ, (A=Ba, La, Sr) to ensure controlled nanoparticle formation and to avoid uncontrolled Ni0 nanoparticle growth apart from the support. Sr,Ni and Ba,Ni–hexaaluminates promote high activity of the catalyst in the dry reforming reaction of CH4, but show fast deactivation if the Ni content is maladjusted in the hexaaluminate framework (y≥0.5). La,Ni–magnetoplumbites display much lower activity accompanied by fast deactivation. The use of very high calcination temperatures (1600 °C) resulting in low specific surface area is detrimental to the activity in the dry reforming of CH4, simultaneously higher hexaaluminate phase content obtained undoes catalytic stability, reasoned by Ni0 nanoparticles produced after reduction cannot be stabilized over surface defects typically found on hexaaluminate platelets calcined at moderated temperatures (<1300 °C). As a result, larger metallic Ni ensembles are built up, selectivity to coke is increased and catalytic stability is compromised.

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