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Creation of heterogeneous catalysts based on hierarchical macrostructures of porous coordination polymers

基于多孔配位聚合物多级宏观结构的多相催化剂的制备

基本信息

批准号：
26870310
负责人：
REBOUL Julien
金额：
$ 2.5万
依托单位：
Kyoto University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Young Scientists (B)
财政年份：
2014
资助国家：
日本
起止时间：
2014-04-01 至 2015-03-31
项目状态：
已结题

项目摘要

The purpose of the research was the creation of new monolithic macrostructures with a hierarchical porosity dedicated to continuous flow catalysis. The targeted structures are made of porous coordination polymers (PCPs), a new class of crystalline materials assembled by organic linkers and inorganic joints at the molecular scale. They are synthesized by applying a method developed in the applicant's group, so-called "coordination-replication", which enables to precisely control the PCP crystallization location through a dissolution-recrystallization process, where a sacrificial metal oxide dissolves and therefore provides the metal cation required to built the PCP crystals. So far, this process was only carried out with metal oxide phases composed of one unique type of metal as sacrificial template, such as pure alumina.In this project, the applicant selected as sacrificial template a mixed metal oxide phase MOx-M’Ox doped with redox active metal centers (M’) or metal oxide phase made of catalytically active transition metals.In this project, the sacrificial template used were vanadium doped alumina aerogels and copper hydroxide macro porous monoliths. Monolithic and polycrystalline macrostructures made of catalytically active PCP crystals were successfully synthesized with different types of organic linkers and characterized.The catalytic activity of these materials are under investigation.

该研究的目的是创造新的整体宏观结构，其具有致力于连续流动催化的分级孔隙率。目标结构由多孔配位聚合物（PCP）制成，这是一类由有机连接体和无机接头在分子尺度上组装的新型结晶材料。它们通过应用在申请人的小组中开发的所谓的“配位-复制”的方法来合成，该方法能够通过溶解-重结晶过程精确地控制PCP结晶位置，其中牺牲金属氧化物溶解并因此提供构建PCP晶体所需的金属阳离子。到目前为止，该方法仅使用由一种独特类型的金属（例如纯氧化铝）组成的金属氧化物相作为牺牲模板进行。在该项目中，申请人选择掺杂有氧化还原活性金属中心（M '）的混合金属氧化物相MOx-M' Ox或由催化活性过渡金属制成的金属氧化物相作为牺牲模板。所用的牺牲模板是钒掺杂的氧化铝气凝胶和氢氧化铜大孔整料。采用不同类型的有机连接剂成功地合成了具有催化活性的PCP晶体的整体和多晶宏观结构，并对其进行了表征，这些材料的催化活性正在研究中。