A Study On The New Synthesis Methods And Application Of Titanium Silicalite-1 (TS-1)

Since TS-1 as a new catalytic material was discovered by EniChem Company in 1983, it attracts a plenty of interests because of its high performance in a series of industrial applications such as phenol hydroxylation and cyclohexanone ammoximation. Besides conventional hydrothermal synthesis, many new synthesis methods appeared with the development of inorganic synthesis techniques, for example, microwave irradiation-assisted synthesis, balling milling method, ion implantation method and chemical grafting method. During the applications of TS-1, it suffers the problems such as the difficulty of separation because of small particles. Generally, preparation of extruded catalysts is an efficient method to solve this problem. However, the addition of binders will affect the catalytic performance of active component. And the strength of extruded catalysts is another obstacle. On the other hand, many researchers propose several other methods for preparing TS-1 zeolites. Although the microwave method was reported in the literatures, it is necessary to study the details and the mechanism. Based on the importance of TS-1 in the catalysis field, the study on TS-1 zeolite is a hot topic and it is important to expand its application.In this work, we studied several aspects about the synthesis methods and the applications of TS-1. Firstly, TS-1 was loaded by direct synthesis on the stainless-steel-net to form an integrated material, which avoids completely the filtration during the preparation of the catalyst. The TS-1 zeolite was successfully coated on the support and was rich in Ti active sites as evidenced by characterizations and using catalytic reaction of probe substrate,1-hexene. The TS-1/stainless-steel-net materials were applied in the continuous reaction of allyl chloride epoxidation. And it showed a potential to the application of the TS-1 in the fixed bed. Secondly, we studied the microwave-assisted synthesis of TS-1 zeolite and its catalytic activity. The synthesis process was investigated to explain the mechanism of crystallization. Thirdly, the fluorine species were introduced into the synthesis of TS-1. The physical and chemical properties and the catalytic performance of resultant TS-1 with fluorine species were investigated to study the influence of the fluorine species. The fluorine species were also introduced into TS-1 via the post-treatment and the chemical grafting method. We found that the fluorine species poisoned the TS-1 catalyst.