金属有机框架ZIF-67基Co@Carbon膜催化反应器设计、制备及其用于丙烷催化脱氢反应过程强化研究

The direct catalytic dehydrogenation of propane to propylene is a reversible equilibrium reaction process. In a fixed-bed reactor, the conversion of propane and the yield of propylene are greatly restricted. In view of the reaction characteristics of propane dehydrogenation to propylene, this project will develop a metal organic framework ZIF-67 based Co@Carbon membrane catalytic reactor for efficient catalytic conversion of propane to propylene, realizing the organic unify of reaction and separation processes. The effect of surface composition and physicochemical properties of the porous alumina supports and preparation methods on the morphology, composition, structure and gas permeability of carbon molecular sieve membranes, ZIF-67@PDA membranes and Co@Carbon membrane reactor are investigated in detail. The studies on the correlation between the microscopic effect like morphology, size, composition, structure and distribution of the Co based catalyst of Co@Carbon membrane reactor and yield of propylene are carried out, revealing the structure-activity relationship of membrane reactor. The interaction, coupling and matching rules between catalytic reaction and membrane separation are discussed in the strengthening process of membrane catalytic dehydrogenation of propane to propylene, providing a reliable basis theoretical research for the development of the catalytic membrane reactor with coupling reaction-separation functionality and its industrial application.

丙烷直接催化脱氢制丙烯是一个可逆平衡反应，在通常的固定床反应器中，丙烷转化率和丙烯的产率受到极大的制约。针对丙烷催化脱氢制丙烯的反应特点，本项目拟开发出金属有机框架ZIF-67基Co@Carbon膜催化反应器用于高效催化转化丙烷制丙烯，实现反应和分离的有机结合。研究多孔氧化铝表面组成、理化性能和制备方法等因素对碳分子筛膜、ZIF-67@PDA膜和Co@Carbon膜反应器的形貌、组成、结构和气体渗透性能的影响；考察Co@Carbon膜反应器Co基催化剂的形貌、大小、组成、结构和分布等因素与丙烯产率的关联性，揭示膜反应器的构效关系；丙烷膜催化脱氢制丙烯的反应强化作用，以及催化反应和膜分离的相互影响、耦合和匹配规律，为开发具有反应分离耦合功能的膜催化反应器及其工业应用提供可靠的理论研究基础。