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Molecular Design of Organic-Inorganic Composite Materials for Catalysis

催化用有机-无机复合材料的分子设计

基本信息

批准号：
02650592
负责人：
SEGAWA Kohichi
金额：
$ 1.22万
依托单位：
Jyouchi Daigaku (Sophia University)
依托单位国家：
日本
项目类别：
Grant-in-Aid for General Scientific Research (C)
财政年份：
1990
资助国家：
日本
起止时间：
1990 至 1991
项目状态：
已结题

项目摘要

Zirconium phosphonates are solid materials typically synthesized in amorphous forms under aqueou conditions by the reaction of a soluble salt of a tetravalent metal and a phosphonic acid or an organophosphori acid :However, it is possible to synthesize many of them as crystalline compounds. Preparation and characterization of two-dimensional zirconium phosphonate derivatives have been investigated. The potential applications of crystalline zirconium phosphonates have significant recent interest. Depending on the R group, different applications for these materials in the field of chromatographic separation, photochemistry, fuel cell, and catalysis are expected. In the case of zirconium phosphates, with the general formula. Zr(O_3POH)_2・nH_2O, the most extensively investigated crystalline zirconium, phosphate is an a layered acid salt, alpha-Zr(O_3POH)_2-H_2O crystallizes in the monoclinic system, as assigned by Troup and Clearfield from their single crystal work. For the zirconium phosp … More honates, however, the twodimensional tetravalent metal plane has a structure essentially similar to the zirconium phosphate structure ; substituted for hydroxyl groups are the desired organic functional groups, oriented away from the basal surfaces in a bilayered fashion in the interlayer region. Therefore, zirconium phosphonate materials can act as a series of modified surfaces, and become accessible for reactant molecules of catalysis.Two composite zirconium phosphonates in single crystal phase have also been investigated and characterized by XRD, ^<13>C-, and ^<31>P-MASNMR. These compounds are lamellar structures comprising zirconium phosphates or organophosphonates. Each layer consists of planes of zirconium bridged through phosphonate groups which altemate above and below the Zr atom planes, oriented away from the basal surfaces in a bilayered fashion in the interlayer region. The catalytic performance over zirconium phosphonates is evaluated by hydrolysis of ethylacetate or by esterification of acefic acid. When the composite zirconium phosphonate is composed with an acidic function and with a hydrophobic function in single crystal phase, the catalytic activity showed a higher activity without swelling of the catalyst in the reaction media. The composite materials become accessible, to any reactant molecule and improve hydrophobicity. Less

磷酸锆是一种固体物质，通常在水条件下由四价金属的可溶性盐与膦酸或有机磷酸反应而合成为无定形。然而，也有可能将它们中的许多合成为结晶化合物。研究了二维膦酸锆衍生物的制备和表征。结晶磷酸锆的潜在应用近年来引起了人们的极大兴趣。根据R基团的不同，这些材料有望在色谱分离、光化学、燃料电池和催化等领域得到不同的应用。在磷酸锆的情况下，用通式。Zr(O_3POH)_2·nH_2O是研究最广泛的结晶型磷酸锆，是一种层状酸盐，α -Zr(O_3POH)_2- h_2o在单斜晶系中结晶，由Troup和Clearfield从他们的单晶工作中得出。然而，对于磷酸锆，二维四价金属平面具有与磷酸锆结构本质相似的结构；取代羟基的是所需的有机官能团，在层间区域以双层方式取向远离基面。因此，磷酸锆材料可以作为一系列修饰表面，并成为反应物分子催化的可利用材料。用x射线衍射（XRD）、^<13>C-和^<31>P-MASNMR对两种单晶复合磷酸锆进行了表征。这些化合物是由磷酸锆或有机膦酸盐组成的层状结构。每一层都是由由磷酸盐基团桥接的锆平面组成的，磷酸盐基团在Zr原子平面的上下交替，在层间区域以双层的方式远离基面。通过乙酸乙酯的水解或乙酸的酯化反应来评价磷酸锆的催化性能。当复合膦酸锆在单晶相中具有酸性功能和疏水功能时，催化活性表现出更高的活性，催化剂在反应介质中不膨胀。复合材料变得易于接触任何反应物分子，并提高了疏水性。少