基于多尺度协同晶化的ZSM-5纳米薄层沸石低成本合成及其催化性能研究

Aiming at the important technologies, such as methanol-to-olefins, methane conversion to aromatics, etc., and to achieve high selectivity, high conversion rate of catalytic reactions and high stability of the catalysts, the multi-scale cooperative synthesis of low-cost ZSM-5 nanosheets will be investigated to reveal the cooperative mechanism of templates during crystallization and the structure-activity relationship between multi-level hierarchy and catalytic performance. It is proposed to reduce the synthesis cost of ZSM-5 zeolite nanosheets by using the cheap templating agents which would match the crystallization rate of the diquaternary ammonium surfactant and stabilize the micelle. On this basis, by changing the acidic properties of ZSM-5 nanosheets, the catalytic lifetime of the catalytic materials will be improved and the application feasibility will be increased. Furthermore, by designing a novel low-cost single quaternary ammonium surfactant as a template, it is expected to obtain a lower synthesis cost ZSM-5 nanosheets. This work will bring the immense advantages of ZSM-5 nanosheets to the fields of petroleum refining, industries of coal chemicals and fine chemicals, providing a theoretical basis for the design and synthesis of high-efficiency catalysts.

针对甲醇制丙烯、甲烷转化制芳烃等炼油向化工转型重要技术，以实现催化反应的高选择性、高转化率和催化剂的高稳定性为目标，围绕ZSM-5纳米薄层沸石的多尺度协同晶化和低成本合成展开研究，揭示其晶化过程中的协同作用机理和多级结构与催化性能之间的构效关系。提出通过筛选与双季铵盐表面活性剂晶化速度相匹配且能稳定胶束的廉价模板剂，以协同晶化的方式降低ZSM-5纳米薄层沸石的合成成本。进一步，通过设计新型的低成本单季铵盐表面活性剂作为模板剂，有望获得更低合成成本的ZSM-5薄层沸石。在此基础上，通过改变ZSM-5纳米薄层沸石的酸性质以改善该催化材料的催化寿命，增加其应用可行性。本课题的工作将有利于发挥ZSM-5纳米薄层沸石在石油炼制、煤化工与精细化工等催化领域中的巨大优势，为高效催化剂的设计合成提供理论依据。

针对甲醇转化、催化裂解制低碳烯烃等炼油向化工转型重要技术，以实现催化反应的高选择性、高转化率和催化剂的高稳定性为目标，本项目首先围绕ZSM-5纳米薄层沸石的多尺度协同晶化和低成本合成展开研究，揭示其晶化过程中的协同作用机理和多级结构与催化性能之间的构效关系。通过筛选与双季铵盐表面活性剂晶化速度相匹配且能稳定胶束的廉价模板剂，以协同晶化的方式大幅降低了ZSM-5纳米薄层沸石的合成成本。进一步，通过在TBAOH-凝胶体系中添加价廉的晶化促进剂，获得了固收率接近90%的纳米薄层ZSM-5沸石，合成成本大幅下降。此外，在无有机模板存在下，通过晶种法并优化合成配方，获得了低成本的短b轴ZSM-5沸石，催化裂解反应性能大幅上升。本课题的工作将有利于发挥ZSM-5薄层沸石在石油炼制、煤化工与精细化工等催化领域中的巨大优势，为高效催化剂的设计合成提供理论依据。