Design of Layered Silicate by Grafting with Metal Acetylacetonate for High Activity and Chemoselectivity in Photooxidation of Cyclohexane

  • Nao Tsunoji
    Department of Applied Chemistry, Graduate School of Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527, Japan
  • Yusuke Ide
    World Premier International (WPI) Research Center, International Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba 305-0044, Japan
  • Yuya Yagenji
    Department of Applied Chemistry, Graduate School of Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527, Japan
  • Masahiro Sadakane
    Department of Applied Chemistry, Graduate School of Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527, Japan
  • Tsuneji Sano
    Department of Applied Chemistry, Graduate School of Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527, Japan

書誌事項

公開日
2014-03-21
資源種別
journal article
DOI
  • 10.1021/am500515p
公開者
American Chemical Society (ACS)

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説明

We succeeded in the immobilization of Ti(IV) acetylacetonate onto interlayer surfaces of a layered silicate HUS-2 (Hiroshima University Silicate-2, Si20O40(OH)4·4[C5H14NO]) and investigated the photocatalytic acitivity of Ti-incorporated HUS-2 toward the partial oxidation of cyclohexane to cyclohexanol and cyclohexanone under solar light irradiation. XRD, SEM/EDX, (13)C CP and (29)Si MAS NMR and UV-vis measurements of Ti-incorporated HUS-2 confirmed that the isolated tetrahedral Ti species were homogeneously immobilized onto silicate sheets via Si-O-Ti covalent bond and acetylacetonate ligands were removed after calcination. Ti-incorporated HUS-2 showed ca. 100% selectivity for partial cyclohexane oxidation and considerably higher yields (cyclohexanol and cyclohexanone) than TS-1, a typical Ti-containing zeolite. Higher yields were obtained when the calcined Ti-incorporated HUS-2 with a larger amount of the grafted Ti were used.

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