表面Cu(0)/Cu(I)比例可控的核壳结构铜基CO2加氢催化剂的研究

项目名称： 表面Cu(0)/Cu(I)比例可控的核壳结构铜基CO2加氢催化剂的研究

项目编号： No.21306118

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 化学工业

项目作者： 岳海荣

作者单位： 四川大学

项目金额： 25万元

中文摘要： CO2催化加氢制低碳醇是CO2资源化利用的重要途径之一。针对铜基催化剂在高温催化加氢等许多工业过程普遍面临的铜晶粒迁移、烧结和铜活性组分价态不稳定引起失活这一核心科学问题，本研究提出采用水热合成和模板剂等方法，构筑表面不同价态铜活性组分稳定及比例可控的壳核结构，通过研究催化剂组成、结构特征及活性位形成机制，调控铜基催化剂的形貌结构和表面Cu(0)和Cu(I)活性位的分布，研究核壳结构铜催化剂在CO2加氢反应的构效关系，弄清催化剂在反应过程中的组织结构和活性位变化规律，确定影响加氢反应催化剂稳定性的主要因素，探明铜基催化剂高温失活机理。拟采用材料制备到构效关系研究再反馈到制备过程的技术路线，指导合成适用于高温、具有双价态铜活性位高效稳定的核壳铜催化剂，从而解决加氢反应铜活性组分烧结和价态不稳定的问题。本研究不仅将拓展CO2加氢反应过程高效稳定铜催化剂的研究，也为常规材料功能化利用提供新途径。

中文关键词： CO2加氢；核壳结构；协同作用；硅酸铜；铜基催化剂

英文摘要： Catalytic hydrogenation of CO2 to lower alcohols is an important approach for the chemical utilization of CO2. The sintering of the copper-based catalysts at high temperature and the unstable surface active copper species with different valence states are the key issues for the copper-based catalysts in many industrial processes, particularly for the hydrogenation reaction. This proposal is about the design of highly efficient and stable core-shell structure multifunctional materials with finely tuned morphologies and active species, and the investigation of the activities and stability in the CO2 hydrogenation reaction. Copper-based catalysts with core-shell structures will be synthesized via hydrothermal synthesis and template-directed methods. On the basis of the characterization of structures and formation mechanism, the morphologies of the catalysts and surface active copper species will be finely tuned, and the structure-activity relationship of the core-shell catalysts in CO2 hydrogenation will be evaluated. Through analysis of the morphologies and the changing regularity of surface active copper species, the facts affecting the long-term stability of the catalysts in the CO2 hydrogenation conditions and high-temperature thermal process will be studied, and the mechanism of the inherent will be proposed.

英文关键词： hydrogenation of CO2；core-shell structure；synergistic effect；silicates；copper catalysts