丙烯直接气相环氧化是全球关注的环氧丙烷绿色合成新路线，其中Au/钛硅分子筛为最有前景实现该反应的催化剂体系。本项目致力于认识和解决Au活性组分在多级孔钛硅分子筛孔道内空间分布和粒径大小的不可控而导致的催化活性和稳定性劣化的瓶颈问题，其同属于负载型多级孔道分子筛催化剂设计过程中的共性难点。通过设计合成介孔贯通的多级孔道TS-1，利用Au前驱物种空间位阻差异及分子筛不同结构性质等因素，发展可控调变Au物种在分子筛微-介孔道内尺寸及空间分布的新方法；耦合原位表征、数学模型等手段，揭示催化剂介尺度结构在溶液及气体氛围中的动态演化规律，建立催化剂介尺度结构的调控机制；结合环氧化性能及结焦动力学等分析，明确介尺度结构对催化剂服役过程的劣化影响机制，阐释Au-Ti双功能催化剂介尺度结构效应的本质。本研究将为负载型分子筛催化剂的理性设计奠定重要的理论和应用基础，助推丙烯气相环氧化工业化进程。

As the novel strategy for the green synthesis of propylene oxide, direct gas-phase propene epoxidation has been a global focus, and Au/titanium silicalite is the most promising catalyst for this reaction. This project aims to understand and solve the bottleneck problem, i.e., the deterioration of catalytic performance resulted from the uncontrollable metal spatial location and size. This is also the common difficulty in the design of supported hierarchical zeolite catalysts. The interconnected titanium silicalite-1 is first designed, and the novel strategy to tune Au size and spatial distribution is developed based on the steric hindrance of various gold precursors and structure of zeolite, etc. In addition, the dynamic evolution law and formation mechanism of mesoscale structure are then established by coupling multi-factors analysis such as in-situ characterization and mathematical modeling. By analyzing the performance of propene epoxidation and coking kinetics, the effect of mesoscale on the deterioration mechanism of catalysts is established and intrinsic nature of structure effect is also elucidated. This project lays solid theoretical and application foundation for the design of supported zeolite catalysts, and is of great significance to accelerate the industrialization of direct gas-phase propene epoxidation reaction.