针对碳基能源转化利用的沸石分子筛催化材料的设计合成

The systemically investigation of highly utilization of carbon resource including petroleum, coal, natural gas, biomass etc. is of great importance for the safety of resource as well as the sustainable development of energy industry in China. The utilization of heavy oil has been one of the most important projects in refine industry since nowadays. Fischer-Tropsch (F-T) synthesis via catalytic transformation of the syngas (H2+CO) to produce liquid fuels has been one of the most used routes for the utilization of coal, natural gas, biomass etc. However, the high selectively product ion of gasoline, diesel as well as kerosene have been one of the most challenges for traditional F-T synthesis. The development of mesoporous zeolites would benefit the refine of heavy oil and increase the selectivity of F-T synthesis. On the other hand, molecular reconstruction reactions including isomerization, reforming etc. are of great importance for the increase the quality of liquid fuels. However, the preparation of the catalytic materials for molecular reconstruction reactions, zeolites with 1-D pores, is still challenged due to its traditional route with low efficiency and high pollution. .Thus, we would systemically investigate new routes for design and prepare zeolites used in refine of heavy oil, F-T synthesis as well as molecular reconstruction reactions in this project. Furthermore, we would study the mechanism for templates and solvents in zeolite crystallization, the synthetic effect of porous structure and catalytic active site at atomic level. Based on these results, we would reveal the basic theory for preparation of zeolites and the principal law for the porous structure and catalytic activity.

为保障我国能源安全和实现能源工业的可持续发展，开展石油、煤、天然气、生物质等碳资源的高效利用技术的研究具有重要意义。重质油的加工是目前以及今后石油炼制面临的重要课题之一，经由合成气(H2+CO)催化转化的费托合成液体燃料是煤、页岩气和生物质等非油基碳资源优化利用的最可行途径之一，而高选择性地合成汽油、柴油和航空煤油组分是提高传统费托合成过程经济性的主要途径。介孔沸石分子筛的应用是提高重质油炼制和调控费托合成产物的关键技术。另一方面，分子重构反应对于提高液体燃料的品质起了非常重要的作用。而适用于分子重构反应的一维沸石分子筛的大规模应用需要进一步优化其制备方法。因此本项目将围绕上述反应所涉及的沸石催化剂材料的设计合成，深入研究分子筛合成过程中的模板作用机制、溶剂作用机制以及孔道结构与原子水平催化中心的系统协同，揭示定向设计沸石分子筛的基础理论以及沸石分子筛的质构性质与催化性能的内在规律。

为保障我国能源安全和实现能源工业的可持续发展，开展石油、煤、天然气、生物质等碳资源的高效利用技术的研究具有重要意义。重质油的加工是目前以及今后石油炼制面临的重要课题之一，经由合成气(H2+CO)催化转化的费托合成液体燃料是煤、页岩气和生物质等非油基碳资源优化利用的最可行途径之一，而高选择性地合成汽油、柴油和航空煤油组分是提高传统费托合成过程经济性的主要途径。按照项目计划书的要求，本项目开展晶体结构、孔道尺寸和构型与催化活性位协同和匹配的双(多)功能多级孔沸石分子筛催化材料的设计，并综合研究沸石晶化和孔道形成机制，催化活性中心组装和构筑方法，尤其是晶体内部介孔孔道的控制，晶面取向和形貌的精确调控，孔道结构与催化中心的协同增强等科学问题。在此基础上使用双功能聚合物模板定向合成介孔沸石分子筛EU-1和具有纳米片层结构的SAPO-11，实现介孔沸石分子筛的多级孔道精确构筑，并研究了分子筛晶体结构和介孔孔道在重质油加工、费托合成以及分子重构等一系列重要化工过程中的应用和催化本质，揭示催化材料质构性质影响催化性能的内在规律；使用核磁共振和紫外-拉曼等谱学表征手段研究，无溶剂合成AlPO-5和A等沸石分子筛过程中的机理，揭示在上述可持续路线合成沸石过程中起始原料的扩散、解聚、有机模板剂的作用、结构单元的产生和缩聚、晶种的溶解活化、晶体生长等机制，发展沸石分子筛的绿色合成路线，设计合成了包括AlPO-5、ZSM-22等一维分子筛在内的绿色合成途径，为一维沸石分子筛在能源转化方面的进一步广泛应用提供技术支撑。