F-T基轻烃芳构化高效催化剂研制与反应过程研究

Fischer-Tropsch synthesis is the key technology of indirect coal liquefaction process, and its subsequent processing determines the process economy to a certain extent. The main products from the existing processing technology for light fraction oil are LPG and naphtha, which is difficult to meet the market and process economic needs. Based on this, this project proposes a new process of catalytic cracking combined with aromatization to produce high value-added aromatic hydrocarbons, aiming at promoting the value of light fraction oil derived from F-T synthesis. At the same time, researches and developments on efficient and Zn anti-loss molecular sieve catalyst was carried out in accordance with the aromatization process, which is the key catalytic process in this scheme. The online supplement and activation of Zn active center will be realized by introducing spinel auxiliary materials with Zn slow-release function. Based on this, we expect to solve the key scientific problems of the structural elucidation, migration and losing patterns, and catalytic mechanism of active sites involved in Zn-containing zeolite catalysts in aromatization reaction. Combining with the exploration on the suitable technologies for aromatization of cracking products from light fraction oil, we can get regularity knowledges and develop efficient catalyst and matching fluidized bed reaction process for aromatization of light hydrocarbons derives from F-T synthesis.

费托合成是煤炭间接液化过程的关键技术，其产品后续加工一定程度上决定了过程的经济性，现有加工工艺对轻质馏分油处理产品为LPG和石脑油，难以满足市场和过程经济需求。基于此，本课题针对费托合成轻质馏分油加工提值问题，提出催化裂解结合芳构化生产高附加值芳烃的处理新工艺，可在提高过程经济性的同时丰富煤间接液化产品方案；同时针对这一方案中的关键催化过程——芳构化反应开展高效、抗活性物种流失的分子筛催化剂及与之相匹配的流化床工艺研发，通过引入具有Zn缓释功能的尖晶石助剂材料，实现Zn活性中心的在线补充和活化。通过本研究，本课题预期解决含Zn分子筛催化剂在芳构化反应中活性中心的结构解析、流失、迁移规律及其催化作用机制等关键科学问题，结合适合费托合成轻质馏分油裂解产物结构特点的芳构化反应工艺探索，获得规律性认识，研发费托基轻烃芳构化高效催化剂及与之匹配的流化床反应工艺。

费托合成产品的深加工、高值化利用是影响煤炭间接液化过程经济性的关键因素。项目围绕F-T合成油高值化利用，提供一条以芳烃为目标产物的轻馏分油加工处理路线，并针对该路线中的关键过程——低碳烃芳构化催化剂及流化床工艺开展研究，旨在通过添加缓释组分的方法，解决含Zn分子筛催化剂用于低碳烃芳构化存在的活性组分流失问题，并发展与之相适应的流化床反应工艺。项目完成预定目标，具体包括：.1）研发了具有高活性、高稳定性、有效减缓抗Zn流失的新型低碳烃芳构化催化剂，系统考察了尖晶石复合分子筛催化剂的制备方法，实现Zn缓释催化剂结构可控合成。.2）认识了催化剂中金属物种存在方式与分子筛孔道限域效应对中间体活性和反应机理的影响规律，揭示Zn缓释催化剂构效关系，阐明了低碳烃芳构化反应及还原气氛分子筛上Zn迁移、流失机制。.3）发展了F-T合成轻油催化裂解技术，并形成与之相匹配的混合低碳烃多级耦合芳构化方案，建立F-T合成产品分级转化处理方案，提供一条以芳烃为目标产品的轻馏分油裂解-芳构化反应路线。.发表高水平期刊Chem. Commun., Chem Catal., Microporous Mesoporous Mater., J. Phys. Chem. C, ChemCatChem论文10篇，申请中国发明专利4件、美国专利1件，其中授权中国发明专利3件、美国专利1件。.