Opanasenko Maksym V, Montanari Erica, Shamzhy Mariya V
Department of Synthesis and Catalysis, J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 18223 Prague 8 (Czech Republic), Fax: (+420) 28658 2307.
Department of Porous Materials, L. V. Pisarzhevskiy Institute of Physical Chemistry, National Academy of Sciences of Ukraine pr. Nauky 31, 03028 Kiev (Ukraine).
Chempluschem. 2015 Mar;80(3):599-605. doi: 10.1002/cplu.201402346. Epub 2015 Jan 8.
Novel layered organic-inorganic materials functionalized with amino groups have been synthesized by using a two-dimensional zeolitic precursor, IPC-1P, prepared by a top-down approach from zeolite UTL. The formation of porous materials containing silsesquioxane linkers covalently bonded to zeolite layers in the interlayer space was confirmed by a variety of characterization techniques (N sorption, XRD, TEM). The textural properties and catalytic behavior of functionalized hybrid materials synthesized by direct pillaring of IPC-1P or by grafting of (3-aminopropyl)silyl groups to the IPC-1P precursor preliminarily pillared with tetraethoxysilane (TEOS) were compared. The use of a mixture of aminosilsesquioxanes and TEOS for pillaring of IPC-1P led to the formation of functionalized materials, which are characterized by excellent textural properties (S =154-435 m g , V =0.336-0.630 cm g ) and provide a 100 % yield of target benzylidenemalononitrile in the Knoevenagel condensation of benzaldehyde and malononitrile.
通过使用二维沸石前驱体IPC-1P合成了用氨基官能化的新型层状有机-无机材料，IPC-1P是由UTL沸石通过自上而下的方法制备的。通过多种表征技术（N吸附、XRD、TEM）证实了在层间空间中形成了含有与沸石层共价键合的倍半硅氧烷连接体的多孔材料。比较了通过IPC-1P直接柱撑或通过将（3-氨丙基）硅烷基团接枝到预先用四乙氧基硅烷（TEOS）柱撑的IPC-1P前驱体上合成的官能化杂化材料的织构性质和催化行为。使用氨基倍半硅氧烷和TEOS的混合物对IPC-1P进行柱撑导致形成官能化材料，其具有优异的织构性质（S = 154 - 435 m²/g，V = 0.336 - 0.630 cm³/g），并且在苯甲醛和丙二腈的Knoevenagel缩合反应中目标苄叉丙二腈的产率为100%。
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