合成气制芳烃新型纳米核壳催化剂的研制与性能研究

项目名称： 合成气制芳烃新型纳米核壳催化剂的研制与性能研究

项目编号： No.21303240

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 崔晓静

作者单位： 中国科学院山西煤炭化学研究所

项目金额： 25万元

中文摘要： 煤基合成气制芳烃具有重要的理论意义和实用价值。目前，常用于合成气制芳烃的催化剂是具有金属活性位和沸石酸性位的双功能催化剂。这些双功能催化剂通常由浸渍法或机械混合法制备，催化剂上双活性位点协同催化效率低。针对上述问题，本项目拟设计和研制一种新型的纳米核壳双功能催化剂，其中核催化剂为金属催化剂，壳为分子筛催化剂，合成气在核上生成甲醇或烯烃，再在壳上转化为芳烃。为了有效耦合核壳催化剂上的两步反应，实现合成气高效转化制芳烃，本项目拟通过多种表征和固定床反应评价，对催化剂制备和反应过程中的科学问题进行研究，具体包括：（1）核催化剂形貌尺寸的调控机制；（2）核催化剂的表面化学性质对壳分子筛生长的作用机制；（3）制备、还原条件对核、壳催化剂的活性位分布的影响规律。本项目的成功实施将为高性能纳米核壳催化剂的设计和研制提供理论和实践借鉴。

中文关键词： C1催化转化；纳米核壳催化剂；壳的限域作用；Cu0和Cu+的催化机制；

英文摘要： Production of aromatic from coal-derived syngas is becoming a highly effective pathway with the diminishment of petroleum resources.The conversion of syngas to aromatics (STA) is usually catalyzed by a bifunctional catalyst,comprising a metal active stie for CO reduction and a shape-selective zeolite acid site.The consecutive-reaction nature of the STA process demands a sequential distribution of the metal sites and zeolite acid sites. Such distribution of the two active sites can be hardly achieved on the reported bifunctional catalysts,since these catalysts are generally prepared by the impregnation or mechanically mixing method.To acquire such desired active site distribution, a novel core-shell bifunctional nanocatalyst is designed in this work.Specifically,the core of the catalyst is a nano-sized syngas-to-methanol or a syngas-to-olefin metal catalyst, while the shell consists of a zeolite which selectively transforms methanols or olefins into aromatics.To fully understand the relationship between the catalyst structure and its catalytic performances,and prepare an effective core-shell nanocatalyst for STA process,systematic investigations will be carried out to elucidate the effect of preparation on the morphology control of the core nanoparticles,the influence of the surface properties of the core on the

英文关键词： C1 chemistry；the nano core-shell catalysts；the confinement effect of the shell；the catalytic roles of Cu0 and Cu+；