多级有序结构柔性颗粒固定床内含湿混合气体热质传递及吸脱附特性

Flexible metal-organic frameworks (MOFs) have promising application in gas separation and capture for it possess a series of unique characteristics such as ordered microporous structure and active adsorption sites, flexible framework and unique breathing phenomenon. This project focuses on the flow, heat and mass transfer and adsorption/desorption characteristics of wet mixed gases containing CO2 in fixed bed packed with flexible MOF particle. And it aims at a deep understanding of the mechanism and behavior of the unsteady flow, transport, adsorption/desorption of wet mixed gases in fixed bed with ordered multilevel pore structure and flexible solid particles under the interaction of heat and mass transfer, adsorption and desorption, and metal-organics framework deformation. The project will launch the study from three levels, namely adsorbent powder, adsorbent particle and fixed adsorption bed. We expect to discover the competitive adsorption mechanism of wet mixed gas and establish the constitutive relation between the adsorption/desorption and micro structure deformation of adsorbent and then, propose a method to determin the micro structure and adsorption site profile of the high effcient adsorbent. A multiscale transport and adsorption/desorption theoretical model of wet mixed gases in fixed bed packed with multilevel pore structure and flexible adsorbent particles will be established. The mechanism and behavior will be clarified for the interaction among heat/mass transfer, adsorption/desorption and fixed bed structure in adsorption and desorption process. The effect of operation condition and geometric parameter on the performance of adsorption/desorption will be obtained for the fixed adsorption beds. Finally, the multilevel optimization method of the fixed bed structure will be proposed based on the synergetics theory. This project will greatly facilitate the development of CO2 separation and capture technology.

柔性金属-有机固体骨架材料（MOFs）具有有序的微孔结构、吸附位点分布和骨架变形及呼吸作用，在CO2等气体分离和捕获中具有重要的应用价值。本项目以含湿CO2混合气体在柔性MOFs颗粒固定吸附床内的流动、热质传递和吸/脱附特性为研究对象，以重点解决含湿混合气体在多级有序孔结构柔性固体颗粒吸附床内热质传递-吸/脱附-骨架变形相互耦合作用下的非稳态流动和传递热物理科学问题为目标，分别开展吸附剂粉末颗粒、吸附剂颗粒、固定吸附床等三个不同层次且相互关联的研究工作。揭示气相组分的竞争吸附机理和规律，获得组分吸/脱附与吸附剂微观结构变形之间的相互作用关系。建立含湿混合气体在多级有序孔结构柔性吸附颗粒堆积固定床内流动及热质传递多尺度的理论模型，阐明热质传递-吸/脱附-吸附床结构变化之间的相互耦合关系，揭示运行参数对吸附床吸/脱附性能的影响规律，提出构建高效固定吸附床的方法。推动CO2分离捕获技术的发展。

柔性金属-有机固体骨架材料（MOFs）具有有序的微孔结构、吸附位点分布和骨架变形及呼吸作用，在CO2等气体分离和捕获中具有重要的应用价值。本项目以含湿CO2混合气体在柔性金属有机骨架材料（MOFs）颗粒固定吸附床内的流动、热质传递和吸/脱附特性为研究对象，分别开展吸附剂粉末颗粒、吸附剂颗粒、固定吸附床等三个不同层次，相互关联的多级有序孔吸附剂材料内热质传递-吸脱附耦合的非稳态流动传递研究工作。基于Material Studio和GCMC方法的模拟及预测，分别获得了常温下经济快速合成AlFu-MOFs和新型含Cu、Mg异质双金属的MOFs的方法；发现了膜扩散阻力及颗粒内扩散阻力是影响骨架材料粉末颗粒内CO2吸附速率的主要因素；揭示了气相组分的竞争吸附机理和规律；基于格子-Boltzmann法建立了混合气体在多级有序孔结构吸附颗粒堆积固定床内流动及热质传递多尺度模型，揭示了运行参数对吸附床吸/脱附性能的影响规律；提出了一种嵌入树形结构流道的吸附反应器的构建方法。研究结果有力的推动CO2分离捕获技术的发展。. 研究成果已在国内外权威学术刊物和国际学术会议发表相关的高水平论文20篇，其中，包含SCI收录论文4篇，EI收录论文7篇，国际会议论文8篇。公开国家发明专利2项。目前已培养博士研究生1名，硕士研究生5名。其中博士生毕业1名，硕士生毕业4名。课题组多次派出课题组成员参加国际和国内学术交流，其中国际学术会议口头报告5次，国内学术会议口头报告4次。完成了项目研究内容和指标要求。