Mesoporous sieves with unified hybrid inorganic/organic frameworks

Mesoporous sieves with unified hybrid inorganic/organic frameworks
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DOI:
10.1021/cm9903935
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发表时间:
1999-11-01
影响因子:
8.6
通讯作者:
Stein, A
Stein, A
中科院分区:
材料科学2区
文献类型:
--
作者:
Melde, BJ;Holland, BT;Stein, A

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合成了由杂化骨架组成的介孔材料,杂化骨架中的无机组分和有机组分具有固定的化学计量比,并且是共价键合的。UOFMN(统一的有机功能化介孔网络)材料的创建采用了合成MCM-41介孔硅酸盐时使用的概念,使用了季铵盐阳离子表面活性剂和双三烷氧基硅基前体,如双(三乙氧基硅基)乙烷(BTSE)或双(三乙氧基硅基)乙烯(BTSEY)。十六烷基三甲基铵(CTA(+))表面活性剂用酸萃取除去,得到了高比表面积的多孔有机硅酸盐骨架,其中硅原子通过乙烷(来自BTSE)或乙烯(BTSEY)桥联。通道呈蠕虫状,直径均匀。与相同条件下制备的MCM-41相比,UOFMN材料具有更好的水热稳定性和更厚的孔壁。用BTSEY制成的产品中的乙烯基团可以被溴化,溴化产品本身作为溴化源是活性的。用X射线衍射仪、氮气吸附、固体Si-29和C-13核磁共振和透射电子显微镜对UOFMN产物进行了表征。
Mesoporous materials have been synthesized that are composed of hybrid frameworks in which inorganic and organic components have a fixed stoichiometry and are covalently bonded. The creation of UOFMN (unified organically functionalized mesoporous networks) materials incorporates concepts employed in the synthesis of MCM-41 mesoporous silicates, making use of a quaternary ammonium cationic surfactant and a double trialkoxysilyl precursor such as bis(triethoxysilyl)ethane (BTSE) or bis(triethoxysilyl)ethylene (BTSEY). The cetyltrimethylammonium (CTA(+)) surfactant is removed by extraction with acid, resulting in a high surface area porous organosilicate framework in which Si atoms are bridged by ethane (from BTSE) or ethylene (BTSEY) groups. The channels are wormlike and uniform in diameter. UOFMN materials are more hydrothermally stable than MCM-41 prepared under similar conditions and have thicker pore walls. Ethylene groups in products made with BTSEY can be brominated, the brominated product itself being reactive as a bromide source. The UOFMN products were characterized by XRD, N-2 adsorption, solid-state Si-29 and C-13 NMR, and TEM.