氨水再生体系二氧化碳解吸强化和氨逃逸抑制的传质选择性调控研究

CO2 captured by ammonia is one of the most effective methods to control greenhouse gas emissions, but it is far away from the industrial application due to the high regeneration energy consumption as well as the ammonia escape. Based on the carbon dioxide desorption in ammonia solution with the selective mass transfer regulation for the ammonia escape restriction and carbon dioxide deorption enhancement, which is focused on the multi-component transport mechanism and selective regulation, the modeling and solution approaches for the gas-liquid two phase multi-component and multi-physics transportation accompanying regeneration chemical reaction will be developed, and the novel approach of the free ammonia restricted by the additives and N-C bond energy weaken by the catalysts is introduced. The the types and proportions of additives and catalyst to enhance the carbon dioxide desorption and restrain the ammonia escape will be achieved by the comparison of additives and catalysts. The metal organic framework will be fabricated by the metallic ion and organic as the precursor for the derivative metal oxide of MOFs, which is the novel packing materials for the strippers. By the experimental test and numerical simulation, the reliable integration of metallic ion and organic base as well as the optimized three dimensional porous configuration for the derivative metal oxide of MOFs, will be recommended to improve the carbon dioxide desorption and restrict the ammonia escape.

氨法捕集CO2是控制温室气体排放的最有效方法之一，但是高再生能耗和氨逃逸问题一直制约其工业应用。项目以氨水再生过程为对象，以CO2解吸强化和氨逃逸抑制的传质选择性调控为目标，重点围绕伴有再生反应的气液两相间多组分输运机理和多组分选择性调控机制构建两个关键科学问题，开发气液两相间跨尺度多物理化学耦合再生反应输运模型和求解方法，提出引入添加剂通过氢键（配位键）固定游离态的氨和催化剂弱化N-C键键能强化CO2解吸的传质选择性调控思路。进行添加剂与催化剂比选，获得提高CO2解吸性能及抑制氨逃逸传质的添加剂与催化剂类型及配比。以金属离子和有机配体制备金属有机骨架材料(MOFs)作为前驱体，移除部分有机配体得到MOFs衍生金属氧化物作为解吸塔填料。并借助实验和数值模拟研究，通过MOFs衍生金属氧化物结构重构，实现CO2解吸强化和氨逃逸抑制。

本项目围绕有再生反应的气液两相间多组分输运机理和多组分选择性调控机制构建两个关键科学问题，开展了深入系统的研究，全面完成了计划书中各项任务，实现了预期目标。针对关键科学问题“伴有再生反应的气液两相间多组分输运机理”，基于双膜理论与拟单相原理，构建了填料塔内部氨水再生体系内气液两相间跨尺度多物理化学耦合再生反应输运模型和求解方法，揭示了微细多孔介质内氨水再生过程中氨逃逸传质与二氧化碳传质驱动力与阻力。针对关键科学问题“多组分选择性调控机制构建”，首次提出了氧化钨作为催化剂同时促进氨水过程中二氧化碳解吸传质和抑制氨逃逸传质，实现了氨水再生过程在多组分输运选择性调控，构建多物理化学耦合作用下的传质选择性调控机制，揭示其选择性调控机理。项目执行期间，共发表学术论文12篇(均为第一标注)，其中SCI论文11篇影响因子总和超过70，中文工程热物理学报一篇。项目执行期间所发表论文中ESI高被引论文1篇，被选为封面论文1篇，项目成果受到国内外学者关注，并培养硕士研究生7人。