Synthesis of Mesoporous Zirconium Organophosphonate Solid-Acid Catalysts

Synthesis of Mesoporous Zirconium Organophosphonate Solid-Acid Catalysts
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介孔有机膦酸锆固体酸催化剂的合成

DOI:
10.1002/ejic.201101064
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发表时间:
2012-06-01
影响因子:
2.3
通讯作者:
Yuan, Zhong-Yong
Yuan, Zhong-Yong
中科院分区:
化学3区
文献类型:
--
作者:
Lin, Xiu-Zhen;Yuan, Zhong-Yong

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以1-羟基乙叉-1,1-二膦酸为偶联分子,十六烷基三甲基溴化铵为模板剂,水热法合成了骨架上含有桥联有机基团的膦酸锆介孔材料。介观结构是虫洞状的,具有702 m2/g的比表面积和3.6 nm的均匀孔径,并且有机膦酸酯基团均匀地整合在所获得的固体的网络中。羟基亚乙基桥联的介孔膦酸锆固体酸催化剂可用于由D-核糖合成甲基-2,3-O-异亚丙基-β-D-呋喃核糖苷,催化活性高,反应速度快,与液体酸HCl或商品化离子交换树脂NKC-9催化剂的催化性能相当。此外,介孔膦酸锆显示出高的稳定性和良好的重复使用性,在五个循环后没有任何催化活性的损失,这表明它们具有工业应用的潜力。
Mesoporous zirconium phosphonate materials with bridged organic groups in the framework were hydrothermally synthesized with 1-hydroxyethylidene-1,1-diphosphonic acid as coupling molecule and cetyltrimethylammonium bromide as template. The mesostructure is wormhole-like with a specific surface area of 702 m2/g and a uniform pore size of 3.6 nm, and the organophosphonate groups are homogeneously integrated in the network of the obtained solids. The hydroxyethylidene-bridged mesoporous zirconium phosphonates can serve as solid-acid catalysts for the synthesis of methyl-2,3-O-isopropylidene-beta-D-ribofuranoside from D-ribose and exhibit high catalytic activity with rapid reaction rate, which are comparable to the catalytic performance when liquid acid HCl or commercial ion-exchange resin NKC-9 is used as catalyst. Furthermore, mesoporous zirconium phosphonates show high stability with good reusability without any loss of catalytic activity after five cycles, which demonstrates their potential for industrial applications.