胺功能化沸石吸附剂载体的结构性质对CO_(2)吸附性能的影响  

Effect of structural properties of amine functionalized zeolite adsorbents support on CO_(2)adsorption performance

作　　者：刘天祥 李蓉[1] 李晶莹[1,2] 马晓迅 LIU Tianxiang;LI Rong;LI Jingying;MA Xiaoxun(School of Chemical Engineering,Northwest University,Xi’an 710069,China;International Science and Technology Cooperation Base of MOST for Clean Utilization of Hydrocarbon Resources,Xi’an 710069,China)

机构地区：[1]西北大学化工学院,陕西西安710069 [2]国家碳氢资源清洁利用国际科技合作基地,陕西西安710069

出　　处：《煤炭学报》2024年第6期2840-2850,共11页Journal of China Coal Society

摘　　要：为了探究胺功能化沸石吸附剂载体的结构性质对其CO_(2)吸附性能的影响并进一步探索出低成本制备高效CO_(2)吸附剂的有效方法,采用不同的后处理方法对MCM–41沸石的孔道结构进行改造,并将四乙烯五胺(TEPA)负载在这些沸石上制备胺功能化吸附剂。利用N_(2)吸脱附、扫描电镜、X射线衍射、红外光谱等方法对沸石载体进行表征,并利用热重分析仪(TGA)对吸附剂的吸附性能进行评价,系统研究了载体的结构性质、活性胺负载量以及吸附温度对CO_(2)吸附性能的影响,计算了吸附剂的吸附动力学和吸附活化能。最后,通过循环吸脱附实验评估了吸附剂的稳定性。结果表明,通过合理设计载体的结构,可以有效提升基于不同吸附原理的吸附剂的CO_(2)吸附性能。微孔沸石对物理吸附过程更有利,而具有宽孔径分布的多级介孔沸石则比微孔沸石在负载TEPA后表现出更好的化学吸附性能。在80℃和15%(体积分数)CO_(2)条件下,经结构改造并负载TEPA的吸附剂(M–N−T60)的最大吸附容量达到4.04 mmol/g。10次吸脱附循环后,其吸附容量仅下降8.4%,表现出良好的循环稳定性能,这表明M–N−T60为一种有望应用于烟气中CO_(2)捕集的吸附材料。In order to investigate the influence of the structural properties of amine functionalized zeolite adsorbents support on their CO_(2)adsorption performance and further explore effective methods for low-cost preparation of efficient CO_(2)adsorbents,different post-treatment methods were used to modify the pore structure of MCM–41 zeolite,and tetra-ethylenepentamine(TEPA)was loaded onto these zeolites to prepare amine functionalized adsorbents.The properties of the zeolite support were characterized using the methods such as N_(2)adsorption-desorption experiment,scanning electron microscopy,X-ray diffraction and flourier transform infrared spectroscopy.The adsorption performance of the adsorbent was evaluated using a thermogravimetric analyzer(TGA).The structural properties of the support,effects of active amine loading and adsorption temperature on CO_(2)adsorption performance were systematically studied,and the adsorption kinetics and activation energy of the adsorbent was calculated.Finally,the stability of the adsorbent was evaluated through cyclic adsorption and desorption experiments.The results indicate that by designing the structure of the support reasonably,the CO_(2)adsorption performance of adsorbents based on different adsorption principles can be effectively improved.The microporous zeolites are more favorable for the physisorption process,while the hierarchical mesoporous zeolites with a wide pore size distribution exhibit a better chemisorption performance than the microporous zeolites after loading with active amines.At 80℃and 15%CO_(2),the maximum adsorption capacity of the adsorbent(M–N−T60)which modified in structure and loaded with TEPA reached 4.04 mmol/g.After 10 adsorption and desorption cycles,the adsorption capacity of M–N−T60 only decreased by 8.4%,demonstrating good cycling stability,indicating that the M–N−T60 is a potential material for capturing CO_(2)from flue gas.

关 键 词：CO_(2)捕集 胺功能化吸附剂 MCM–41沸石 后处理改性 循环稳定性 

分 类 号：X511[环境科学与工程—环境工程] X383