DEVELOPMENT OF HIGH PERFORMANCE INTEGRATED CATALYSTS FOR SUSTAINABLE CHEMICAL TRANSFORMATION SYSTEMS

可持续化学转化系统的高性能集成催化剂的开发

• 批准号: 18360389
• 负责人: KANEDA Kiyotomi
• 金额: $ 11.12万
• 依托单位: Osaka University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2006
• 资助国家: 日本
• 起止时间: 2006 至 2007
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-18360389/
• 关键词: green chemistry; integrated catalysts; hydrotalcite; montmorillonite; hydroxyapatite; solid acid; dehydrogenation; hydration; 炭素-炭素結合形成反応; 固体酸触媒; 1,4共役付加反応; 固体塩基触媒

In this research project, we aimed development of high performance integrated catalysts for environmentally-friendly and sustainable materials conversion systems. The target reactions are (1) oxidation reactions using molecular oxygen and/or water, and (2) selective carbon-carbon bond formation reactions, which are highly important for synthesis of finechemicals. We have developed novel nanostructured heterogeneous catalysts capable of cooperative activation by several active species, using inorganic crystallites, e. g., hydroxyapatites (HAPs), hydrotalcites (HTs), and montmorillonites (monts), as unique supports. As for the alcohol oxidation, RuHAP functionalized Fe_2O_3 nanoparticles was prepared, which showed extremely high activity fort aerobic alcohol oxidation and also acted as magnetically recoverable catalyst. Furthermore, highly active HT catalyst for conversion of cyclohexanol to cyclohexanone, which is known as difficult oxidation, could be developed. Recent interest in the … More alcohol oxidation has been dehydrogenation without using any oxidants. The Ag/HT catalyst could be extremely high activity for the dehydrogenation of various alcohols. The surface basicity of the HT and the Ag nanoparticles formed on the HT showed the concerted activation of alcohols and generated hydrogen quatitatively. Utilities of the HT catalysts were expanded to hydration of nitrile to amide using vanadium supported HT. Interestingly, acidic clay materials of montmorillonites could be used as solid acid catalysts having protons or various metal cations. These solid acids could catalyze addition reaction of various nucleophiles to olefins forming various C-C, C-O, and C-N bonds.These integrated catalysts can be easily prepared and exhibit outstanding performances, which open a new avenue for sustainable green organic syntheses. The prominent catalyst behavior for the above transformations is focused in relation to the concerted functions between the surface properties of the inorganic crystallites and the metal active species. Less

在本研究项目中，我们的目标是开发用于环境友好和可持续材料转化系统的高性能集成催化剂。目标反应是（1）使用分子氧和/或水的氧化反应，和（2）选择性碳-碳键形成反应，这对于精细化学品的合成是非常重要的。我们已经开发了新型的纳米结构的非均相催化剂，能够协同活化的几个活性物种，使用无机微晶，如。例如，在一个实施例中，羟基磷灰石（HAP）、水滑石（HT）和蒙脱石（蒙茨）作为独特的载体。在醇氧化方面，制备了RuHAP功能化的Fe_2O_3纳米粒子，它对醇的好氧氧化表现出极高的催化活性，并可作为磁可回收催化剂。此外，可以开发用于将环己醇转化为环己酮的高活性HT催化剂，这被称为难氧化。最近对 ...更多信息 醇氧化是在不使用任何氧化剂的情况下脱氢。Ag/HT催化剂对各种醇的脱氢反应都有很高的活性。HT的表面碱性和在其上形成的Ag纳米粒子表明醇类协同活化并产生氢季铵盐。HT催化剂的用途被扩展到使用钒负载HT的腈水合成酰胺。有趣的是，蒙脱石的酸性粘土材料可用作具有质子或各种金属阳离子的固体酸催化剂。这些固体酸可催化各种亲核试剂与烯烃的加成反应，形成各种C-C、C-O、C-N键，且制备简单，性能优异，为可持续的绿色有机合成开辟了新的途径。上述转化的突出催化剂行为集中在无机微晶的表面性质和金属活性物种之间的协调功能。少

项目成果

Magnetically recoverable heterogeneous catalyst: palladium nanocluster supported on hydroxyapatite-encapsulated g-Fe2O3 nanocrystallites for highly efficient dehalogenation with molecular hydrogen

磁性可回收多相催化剂：羟基磷灰石封装的 g-Fe2O3 纳米微晶上负载的钯纳米团簇，用于分子氢高效脱卤

• 发表时间: 2007
• 期刊: Green Chemistry 9
• 作者: Takayoshi;Hara
• 通讯作者: Hara

アルコール脱水素反応におけるハイドロタルサイト固定化銅および銀ナノ粒子の触媒特性

水滑石固定铜银纳米粒子在乙醇脱氢反应中的催化性能

• 发表时间: 2007
• 作者: Kiyotomi;Kandea;H. Tabata;M.Ehara;水垣 共雄;武次徹也;M.Ehara;田畑仁;水垣 共雄;T.Taketsugu;田畑仁;満留 敬人;M.Ehara;武次徹也;海老谷 幸喜;田畑仁;江原正博;武次徹也;三上 輔祐
• 通讯作者: 三上 輔祐

テトラヘドラルパラジウムナノクラスター生成機構のin-situ時間分解XAFSによる解明

使用原位时间分辨 XAFS 阐明四面体钯纳米团簇的形成机制

• 发表时间: 2007
• 作者: Kiyotomi;Kandea;H. Tabata;M.Ehara;水垣 共雄;武次徹也;M.Ehara;田畑仁;水垣 共雄;T.Taketsugu;田畑仁;満留 敬人;M.Ehara;武次徹也;海老谷 幸喜
• 通讯作者: 海老谷 幸喜

Creation of monomeric La complexes on apatite surfaces and their application as heterogeneous catalysts for Michael reactions

• DOI: 10.1039/b512030f
• 发表时间: 2006-01
• 期刊: New Journal of Chemistry
• 影响因子: 3.3
• 作者: K. Mori;M. Oshiba;Takayoshi Hara;T. Mizugaki;K. Ebitani;K. Kaneda

Efficient C-N Bond Formations Catalyzed by a Proton-Exchanged Montmorillonite as a Heterogeneous Bronsted Acid

质子交换蒙脱土作为多相布朗斯台德酸催化有效的 C-N 键形成

• 发表时间: 2006
• 期刊: Organic Letters 8
• 作者: Yoko;Fujie;NORIMATSU;Ken MOTOKURA;Kohki EBITANI;Noriaki FUJITA;Kohki EBITANI;Takayoshi HARA;Ken MOTOKURA
• 通讯作者: Ken MOTOKURA