4.5 Article

Polyoxometalate-nano Gold Hybrid Mesostructured Catalyst for Green Cyclohexene Epoxidation

Journal

CURRENT ORGANIC CHEMISTRY
Volume 21, Issue 25, Pages 2585-2596

Publisher

BENTHAM SCIENCE PUBL LTD
DOI: 10.2174/1385272821666170420155632

Keywords

Gold nanoparticles; polyoxometalates; SBA-15; hybrid mesoporous materials; nanomaterials; cyclohexene epoxidation; molecular oxygen

Funding

  1. Zhejiang Province Natural Science Foundation [Y4080247]
  2. Natural Science Foundation of China [21376213]
  3. Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology [K002]

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Background: The design of a highly active catalyst is a key point in olefins epoxidation. Recently, polyoxometalates have received an increasing interest in selective oxidation of organic compounds. Their scope as nanoparticle carriers is of immense importance as the high anionic charge associated with them prevents sintering of the nanoparticles which is a major issue related to nanoparticle based catalysts thus increasing the stability of the catalyst. Objective: We have immobilized Na9PMo11O (39)(PMo11) and gold nanoparticles on chloropropyltriethoxysilane functionalized SBA-15 mesoporous material. We investigated the molecular oxygen activation ability and stability of this heterogeneous hybrid catalytic system for green epoxidation of cyclohexene under mild reaction conditions. Method: PMo11 was prepared according to the literature, while PMo11/CPTES-SBA-15, Au/CPTES-SBA-15 and Au/PMo 11/CPTES-SBA-15 were prepared by wet deposition method. The catalytic performance was evaluated in a PTFE lined autoclave and analysis was done by gas chromatography. Results: Cyclohexene epoxidation was carried out on different heterogeneous catalytic systems which included polyoxometalate and CPTES-SBA-15 support, nano gold and CPTES-SBA-15 support and the hybrid material Au/PMo11/CPTES-SBA-15 with varying amounts of doped nanogold. All the samples showed good conversion of cyclohexene and significant selectivity for oxidized products with molecular oxygen as an oxidant under mild conditions. 1 % Au/PMo11/CPTES-SBA-15 delivered 48.1 % conversion and 35.9 % selectivity to epoxide. Conclusion: The CPTES-SBA-15 supported Au/PMo11 hybrid catalytic system demonstrated relatively high catalytic activity and selectivity for the green epoxidation of cyclohexene with molecular oxygen as an oxidant under mild reaction conditions. The hybrid catalyst was regenerated and reused for three cycles without compromising the catalytic performance.

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