Catalytic Cracking of Methyl tert-Butyl Ether to Isobutene over Br?nsted and Lewis Acid Sites on Solid-state Molybdenum Sulfide Clusters with an Octahedral Metal Framework
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  • 作者:Satoshi Kamiguchi ; Yasunari Seki ; Akiharu Satake…
  • 关键词:Molybdenum sulfide cluster ; Chevrel phase ; MTBE cracking catalyst ; Br?nsted and Lewis acid ; Bifunctional catalyst
  • 刊名:Journal of Cluster Science
  • 出版年:2015
  • 出版时间:May 2015
  • 年:2015
  • 卷:26
  • 期:3
  • 页码:653-660
  • 全文大小:509 KB
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  • 作者单位:Satoshi Kamiguchi (1) (2)
    Yasunari Seki (3)
    Akiharu Satake (3)
    Kazu Okumura (4)
    Sayoko Nagashima (5)
    Teiji Chihara (5)

    1. Advanced Catalysis Research Group, RIKEN Center for Sustainable Resource Science, 2-1 Hirosawa, Wako, Saitama, 351-0198, Japan
    2. Organometallic Chemistry Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama, 351-0198, Japan
    3. Faculty of Science, Tokyo University of Science, Kagurazaka, Shinjuku-ku, Tokyo, 162-8601, Japan
    4. Faculty of Engineering, Kogakuin University, Nakano-machi, Hachioji, Tokyo, 192-0015, Japan
    5. Graduate School of Science and Engineering, Saitama University, Shimo-Okubo, Sakura-ku, Saitama, Saitama, 338-8570, Japan
  • 刊物类别:Chemistry and Materials Science
  • 刊物主题:Chemistry
    Catalysis
    Inorganic Chemistry
    Physical Chemistry
  • 出版者:Springer Netherlands
  • ISSN:1572-8862
文摘
Solid-state molybdenum sulfide clusters with an octahedral metal framework, the Chevrel phases, are applied to the catalytic cracking of methyl tert-butyl ether (MTBE) to yield isobutene. The copper salt of the nonstoichiometric sulfur-deficient cluster, Cu x Mo6S8?em class="EmphasisTypeItalic">δ (x?=?2.94 and δ?≈?.3), after storing in air, is thermally activated in a hydrogen stream, followed by the reaction with MTBE. Two kinds of catalytically active sites develop depending on the activation temperature: one developed at 100-00?°C is a Br?nsted-acidic hydroxo ligand on the copper cation while the other developed at 350-00?°C is a Lewis-acidic coordinatively unsaturated molybdenum atom with a sulfur-deficient site. A nonstoichiometric sulfur-deficient neutral cluster Mo6S8?em class="EmphasisTypeItalic">δ (δ?≈?.4) also catalyzes the cracking reaction when activated at 400?°C.

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