Study On The Synthesis, Characterization Of New Type Of Complex Pallidiunm Catalysts Supported On The Zirconium (Phosphonate-Phosphate) Containing N, P Ligands Coated On TiO₂ Or ZrO₂ And Their Catalytic Property Of Carbonylation

We can use the hydrogenation, oxidation, especially the carbonylation including hydroformylation catalyzed by transition-metal homogeneous phase complex catalyst to product thousands of chemical products. This is a type of the most promising catalytic reaction for developing the green-chemical 'atomic economy' reaction. The separation, recovery and reuse of these transition-metal catalyst are the biggest obstacle, at the same time , these are the research focus in the field of organic catalyst in recent years. At present, one way of resolving the problem is the or heterogenization of the homogeneous catalysis, namely, loading to maintain the functional advantage of the original homogeneous phase catalyst and reduce or eradicate the draining of the transition metal to realize the reuse of catalyst and reduce the cost of production. The reaction is easily operated and it can easily utilized in the process of industrialization to improve economic benefit and reduce the pollution of the environment. Moreover, after the process of the homogeneous phase complex catalyst, 'effect of polymer' and 'microenvironment effect' would improve the catalytic ability of the catalyst.Zirconium hydrogen phosphate, Zirconium hydrogen phosphite and o zirconium phosphonate are a kind of fine stratified material, with the fixed sandwich and bigger surface area, water-insoluble and organtic-dissolvent and having the ability of withstanding acidity and alkalinity, a higher chemical stability, thermal stability and mechanical strength. The typical a -Zirconium hydrogen phosphate, zirconium phosphonate and mixed zirconium(phosphate -phosphonate) have hundreds m2/g surface area, and the distance of theinterpass can be modified through absorption, insertion, intercalation, fostoon, supportance or bonding connection with a certain size of organic group and then introduce the different active groups or active center on the basis of well-stabile framework of a -Zirconium hydrogen phosphate to produce ionic sieve of different purpose, catalyst and catalytic carrier. Our research group have eerily carried out the research in the field of mixed zirconium (phosphate-phosphonate) functionally in our country and we first put the result of the research of organtic-inorgantic mixed zirconium phosphate catalyst functionally into the research of the transition metal supported complex catalyst. We first prepare a serious of mixed zirconium (phosphate -phosphonate) catalyst carriers having organic lateral chain with coordinating group such as O, N, P and so on, including organic lateral chain with amine derivatives, multiamine derivatives, amino acid derivatives, the mixed zirconium (phosphate-phosphonate) catalyst carrier of the organic with Ph2P-N group derivatives and Ph2P-CH2-N group derivatives and relevant transition-metal palladium catalyst. This supported complex catalyst has highest catalytic activities in hydrogenation and a certain activity of carbonylation and the better effect of reuse.The reactive center of the heterogeneous catalytic reaction mainly lies in the contacted space between the catalytic surface and dissolvent and bottom, so the functional groups having catalytic effect on the surface of catalyst are the main active center in the catalytic reaction. To make use of the catalytic effect of the functional groups, we should try our best to put the functional groups into the surface of catalyst.The author use the olyaminoethylphosphonic acid as the organic phosphoric acid original materials offering organic lateral chain including N and TiO2 and ZrO2 as elementary carriers, and envelop the zirconium (polyaminoethylposphonate-phosphate) on the surface of the metal oxides powder. We firstly prepare 14 TiO2 with different coating ratio and 4 ZrO2 carriers which surface coated by zirconium(polyaminoethyiposphonate-phosphate). On the process of the synthesis of the original materials of polyaminoethylposphonate, we attempt to use 31P NMR and 13C NMR to monitor this process and explain the rationality of the preparation of pol...