Dry Gel Conversion Method for the Synthesis of Organic–Inorganic Hybrid MOR Zeolites with Modifiable Catalytic Activities
Dry Gel Conversion Method for the Synthesis of Organic–Inorganic Hybrid MOR Zeolites with Modifiable Catalytic Activities
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DOI：
10.1021/cm3023538
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发表时间：
2012-11
影响因子：
8.6
通讯作者：
Dan Zhou;Xinhuan Lu;Jun Xu;Anan Yu;Jiyang Li;F. Deng;Q. Xia
中科院分区：
文献类型：
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作者：
Dan Zhou;Xinhuan Lu;Jun Xu;Anan Yu;Jiyang Li;F. Deng;Q. Xia
干凝胶转化（DGC）技术首次应用于有机-无机杂化铝硅酸盐沸石的合成。采用DGC法合成了具有MOR结构的亚甲基桥式有机-无机杂化沸石，不添加有机添加剂，通过粉末XRD、FTIR、固态Si-29、C-13、Al-27 MAS NMR、SEM、元素分析、XRF、XPS和N-2吸附等技术对其进行了结构表征。本文首次报道了通过不同的改性处理，合成的亚甲基桥式杂化沸石可以成功地获得优异的催化活性。将Co2+交换杂化沸石应用于烯烃与空气的环氧化反应，获得了良好的转化率和选择性。特别是，亚甲基桥化沸石可以用发烟硫酸磺化，形成酸性的MOR-SO3H催化剂，对环己酮和乙二醇的酸催化缩合反应表现出很高的催化活性。该方法将成为制备有机-无机杂化沸石或相关分子筛催化剂的一条潜在途径。
Dry gel conversion (DGC) technique is first applied in the synthesis of organic-inorganic hybrid aluminosilicate zeolites. By using the DGC method, methylene-bridged organic-inorganic hybrid zeolites with an MOR topology are synthesized without organic additive, which are structurally characterized by powder XRD, FTIR, solid-state Si-29, C-13, Al-27 MAS NMR, SEM, elemental analysis, XRF, XPS, and N-2 adsorption techniques. This work first reports that thus-synthesized methylene-bridged hybrid zeolites can be successfully bestowed with excellent catalytic activities through different modification treatments. Co2+-exchanged hybrid zeolites are applied in the epoxidation of alkenes with air to achieve good conversions and selectivities. Especially, methylene-bridged hybrid zeolites can be sulfonated with fuming sulfuric acid to form acidic MOR-SO3H catalyst, which exhibits highly catalytic activity for the acid-catalyzed condensation reaction of cyclohexanone and glycol. This method will be one potential route for the fabrication of organic-inorganic hybrid zeolite or related molecular sieve catalysts.