合成气直接制低碳烯烃的催化基础

Lower olefins are considered as building blocks in the chemical industry. The production of lower olefins via a non-oil-based processes is beneficial to the diversification of energy supply and application. It has significant strategic importance on optimizing industrial structure and ensuring national energy security. The direct conversion of syngas into lower olefins via the Fisher-Tropsch synthesis (FTO) over Fe-based catalyst has an attractive prospect due to its simple process, which can operate in a wide range of H2/CO without water gas shift (WGS) reaction unit. This work focus on the formation and evolution of active sites, catalytic mechanism of FTO, the influence of promoters on the crystal structure and local environment of active sites, as well as support effect, all of which play important roles in catalytic performance of FTO reaction. We aim to promote the catalytic performance through coupling the reaction rate of CO hydrogenation and WGS, based on the research on the transformation of active phase at different stages and its regulatory mechanism. Ultimately, an efficient and stable Fe-based catalyst for FTO process as well as a controllable preparation method is obtained. This research will give direction for catalyst rational design and further industrial application for lower olefins synthesis.

低碳烯烃在化学工业中占有重要地位，非石油路线制低碳烯烃技术的应用有利于我国能源和资源利用的多样化，对于优化产业结构、保障我国能源安全具有战略意义。基于Fe系催化剂的合成气直接法制低碳烯烃工艺（FTO）可在较宽H2/CO范围操作，无需水汽变换单元，工艺流程相对简单，具有良好的发展前景。本项目围绕合成气直接法制低碳烯烃工艺中的关键科学问题，重点研究Fe基催化剂的活性中心形成机理及相态演变过程，揭示FTO反应的催化机理；阐明助剂对活性物种结构、相态、化学环境和催化性能的调变和促进机制；获得载体效应对活性组分表面行为和FTO反应性能的影响规律；通过诱导期活性组分相态转变规律和调控机制的研究，提升催化性能，促进反应过程中CO加氢与水汽变化反应速率的耦合。最终获得高效、稳定的FTO工艺Fe基催化剂及可控制备方案，形成基于Fe基催化剂的FTO反应催化理论体系，为催化剂的理性设计和工艺开发提供理论基础。

非石油路线制低碳烯烃技术有利于我国能源的多样化和能源安全。基于Fe系催化剂的合成气直接法制低碳烯烃工艺（FTO）可在较宽H2/CO范围操作，无需水汽变换单元，工艺流程相对简单，具有良好的发展前景。本项目围绕合成气直接法制低碳烯烃工艺中的关键科学问题，重点研究Fe基催化剂的活性中心形成机理及相态演变过程，揭示FTO反应的催化机理；阐明助剂对活性物种结构、相态、化学环境和催化性能的调变和促进机制；获得载体效应对活性组分表面行为和FTO反应性能的影响规律。.项目发表论文11篇，2篇被遴选为封面论文，申请中国发明专利4项。举办APEC“清洁煤化工技术传播和推广研讨会”。和美国南伊利诺伊大学，澳大利亚CSIRO、同辐中心，英国阿伯丁大学在费托合成方面开展了联合研究。