Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2023-03-27 , DOI: 10.1016/j.micromeso.2023.112570 Qiang Yu , Wenna Zhang , Junjie Li , Wen Liu , Yanan Wang , Weifeng Chu , Xinbao Zhang , Longya Xu , Xiangxue Zhu , Xiujie Li
Although FAU zeolites have been widely used as absorbents for volatile organic compounds (VOCs) removal, preparation of high-silica FAU zeolite to expand its application under high humidity is still a big challenge. Here, two high-silica FAU zeolites were successfully prepared through the controllable framework modulation strategy. By carefully matching the degrees of dealumination and Si-insertion, the zeolite (FAU-H) with an ultra-high SiO2/Al2O3 ratio of 957 was obtained. FAU-H exhibited similar high adsorption capacities of VOCs (e.g. m-xylene and toluene) under dry and humid conditions, more importantly, its adsorption capacity of m-xylene was 25% higher than the industrial high-silica FAU zeolite (HSZ-390HUA) from Tosoh Corporation. When the dealumination degree was mismatched with that of Si-insertion, imperfect FAU-M (SiO2/Al2O3 = 108) with the existence of some defect sites was obtained that becomes a good candidate for the adsorption removal of small VOCs molecules (e.g. isopropanol). The moderate interaction between VOCs and zeolite framework is proved a key factor for small molecules adsorption on basis of the DFT calculations. Moreover, the fitted kinetic models, desorption tests, and adsorption−desorption cycling tests proved the good regenerability of FAU-H and FAU-M. Therefore, the proposed high-silica FAU zeolites are promising adsorbents for VOCs removal.
中文翻译:
可控骨架调制高硅FAU沸石用于高湿条件下VOCs吸附
尽管FAU沸石已被广泛用作去除挥发性有机化合物(VOCs)的吸收剂,但制备高硅FAU沸石以扩大其在高湿度下的应用仍然是一个很大的挑战。在这里,通过可控骨架调制策略成功制备了两种高硅 FAU 沸石。通过仔细匹配脱铝和 Si 插入的程度,沸石 (FAU-H) 具有超高 SiO 2 /Al 2 O 3获得了 957 的比率。FAU-H在干湿条件下对VOCs(如间二甲苯和甲苯)表现出相似的高吸附能力,更重要的是,其对间二甲苯的吸附能力比工业高硅FAU沸石(HSZ-390HUA)高25% ) 来自东曹公司。当脱铝程度与硅插入程度不匹配时,不完善的FAU-M (SiO 2 /Al 2 O 3 = 108) 获得了一些缺陷位点的存在,成为吸附去除小 VOCs 分子(例如异丙醇)的良好候选者。基于 DFT 计算,VOC 与沸石骨架之间适度的相互作用被证明是小分子吸附的关键因素。此外,拟合动力学模型、脱附试验和吸附-脱附循环试验证明了FAU-H和FAU-M具有良好的再生性。因此,所提出的高硅FAU沸石是很有前途的VOCs去除吸附剂。