整体式TS-1催化剂的设计合成及其强化传热机理研究

Propene oxide (PO) is an important chemical resource, of which the present routes produce much pollution (Chlorohydrin route) or co-products (Halcon route). Epoxidation of propene with H2O2 over TS-1 to produce PO (HPPO route) is the most possible environmentally benign alternation for the present ones. However, the exotherm of this route is very high, and cannot diffuse outside the catalyst immediately, which will accelerate side reactions and lead to a quick deactivation of the catalyst. In this project, to get rid of the problem of low heat transfer rate in the catalyst, a kind of monolithic TS-1 catalysts with high heat transfer properties will be prepared by supporting TS-1 with high catalytic performance on metallically monolithic supports or metallic microfibers. The relationship between heat transfer coefficient and structure of catalyst will be established, and the influence of the heat transfer properties on the PO selectivity and stability will be discussed by studying the structure, physical chemistry properties, catalytic performances and heat transfer property of the monolithic TS-1 catalyst. This research will provide gist for the catalyst engineering.

环氧丙烷（PO）是一种重要的有机化工原料，其现有生产技术存在环境污染严重（氯醇法）、联产物多（共氧化法）等问题，钛硅分子筛TS-1催化丙烯/H2O2环氧化制PO（HPPO工艺）是最有可能替代现有PO生产技术的绿色工艺。然而，由于该工艺强放热，大量热量不能及时移出催化剂床层，加速副反应进行，导致催化剂失活。本项目拟通过在金属材质的整体式载体或金属微纤维上负载高活性TS-1，研制一种具有高传热性能的整体式TS-1催化剂，解决催化剂内部热量传递慢的问题。通过对整体式催化剂结构、物化性质、催化性能、传热性能的研究，构建传热系数与催化剂结构的关系，探讨传热性能对PO选择性及催化剂稳定性的影响，为催化剂工程化提供依据。

环氧丙烷（PO）及环氧丁烷（BO）是重要的有机化工原料，其现有生产技术存在环境污染严重或联产物多等问题，钛硅分子筛TS-1催化烯烃/H2O2环氧化制环氧化物是最有可能替代现有生产技术的绿色工艺。然而，由于该工艺强放热，大量热量不能及时移出催化剂床层，加速副反应进行，导致催化剂易失活。本项目以金属材质的整体式载体及金属微纤维负载高活性TS-1分子筛进行强化传热，改善催化剂在烯烃环氧化反应中的稳定性。首先，研究了整体式载体及金属微纤维结构优化及表面处理对TS-1负载量的影响；其次，研究了负载条件对负载量的影响；再次，将负载TS-1的整体式催化剂用于丙烯及丁烯环氧化反应，考察其催化性能，并与常规挤条催化剂对比；最后，通过计算模拟了整体式催化剂与挤条成型催化剂床层温度分布，证明整体式催化剂的强化传热效果。在本项目的经费支持下，发表相关SCI收录国外期刊论文4篇，申请中国发明专利6项，授权中国发明专利3项，培养并毕业硕士研究生5名，在读博士研究生2名，在读硕士研究生3名，包括外籍硕士研究生1名。本项目的研究为工业应用催化剂在改善催化性能方面提供了新途径。