高级检索

    Si/Al物质的量比对十二元环沸石拓扑结构影响及其CO2吸附性能

    Influence of Si/Al ratio on topological structure of twelve-membered ring zeolite and its CO2 adsorption performance

    • 摘要: 为应对温室气体排放带来的负面效应,CO2捕集技术成为社会关注焦点。其中固体吸附工艺因低能耗和工艺简单等特点而成为新一代备选技术,因此设计合适的固体吸附剂成为该工艺的技术关键。近年来,高传质效率和高选择性的十二元环孔道沸石,在气体分离领域展现出较大的应用潜力。其中一维十二元环孔道的ECR-1和MOR沸石具备相似的结构单元,可以通过调节沸石结晶过程中的原料Si/Al物质的量比和过碱度,实现ECR-1和MOR两晶相之间的过渡转变以及形貌变化;试验通过XRD、SEM和TEM等方法验证材料的结构和形貌变化。在过碱度为0.33、Si/Al物质的量比为7的条件下,利用浆料结晶的新途径成功制备出纤维状的ECR-1结构,在此基础上继续增加Si/Al可成功合成直径为60~100 nm的MOR沸石纤维杆,其比表面积达到425.58 m2/g;随着Si/Al物质的量比的进一步上升样品变为颗粒状形貌。在单组份CO2动态吸附测试中,发现ECR-1在298 K,105 Pa的条件下CO2动态吸附容量达3.98 mmol/g;并且考虑烟气吸附的实际工况,进行含水的模拟烟气条件测试,发现纤维状形貌的ECR-1和MOR沸石对水气的影响较为敏感,相对干燥条件CO2吸附量在潮湿情况降低15%,而中等颗粒状MOR展现出4%~5%下降;结合Si/Al物质的量比和形貌因素考察了H2O对CO2吸附抑制效应,纤维状形貌导致增加的侧边八元环孔道可能是主要影响因素;同时也测试ECR-1的稳定循环性。

       

      Abstract: In response to the negative effects of greenhouse gas emissions, CO2 capture technologies are increasingly emphasized. Due to low energy consumption and operational simplicity, solid adsorption processes are regarded as promising candidates for next-generation technologies, which means that solid adsorbent has become the technical key of this process. Twelve-membered ring pore zeolites show great application potential in the field of gas separation due to their high mass transfer efficiency and high selectivity. Since the one-dimensional twelve-membered ring pores of ECR-1 and MOR zeolites have similar structural units, so by adjusting the raw material Si/Al ratio and super alkalinity, the transition between the two crystal phases and morphological changes can be achieved. The changes are verified by XRD, SEM and TEM methods. Slurry crystallization, a new preparation route, prepared a fibrous ECR-1 structure under the conditions of an over alkalinity of 0.33 and a Si/Al ratio of 7. On this basis, further increasing the Si/Al ratio can successfully synthesize MOR zeolite fiber rods with a diameter of 60-100 nm and a specific surface area of 425.58 m2/g. As the Si/Al ratio further increases, the sample becomes granular. In dynamic CO2 adsorption tests, the CO2 adsorption capacity of ECR-1 is observed to reach 3.98 mmol/g at 298 K and 1 bar. Furthermore, considering the actual working conditions of flue gas adsorption, adsorption tests are conducted using simulated flue gas containing water. It is found that compared with dry conditions, the CO2 adsorption capacity of fibrous zeolite decreased by 15%, and the MOR granules decreased by 4%~5%, indicating that the fibrous zeolite is more sensitive to the influence of water vapor. The inhibitory effect of H2O on CO2 adsorption is investigated by combining Si/Al ratio and morphology factors, indicating that the exposed 8-membered ring channels of the fibrous morphology may be the main factor for the decrease in adsorption capacity; the stable cyclic performance of ECR-1 is also tested.

       

    /

    返回文章
    返回