Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2022-06-25 , DOI: 10.1016/j.micromeso.2022.112085 Binghua Zhu , Yu Li , Zhicheng Yan , Zhengquan Yang , Xiaowei Wu , Tian Gui , Yuqin Li , Fei Zhang , Xiangshu Chen , Hidetoshi Kita
The growth process of chabazite seed crystal transformed into chabazite zeolite membrane in an organic template-free and fluoride-containing synthesis gel was investigated in details. The characterization results showed that the formation process of organic template-free chabazite zeolite membrane included the processes of seed crystal dissolution and chabazite crystal reconstruction. In the first process of seed dissolution into amorphous, the secondary building units (D6Rs) of CHA framework were completely destroyed except for the presence of a small number of 4Rs. While the amorphous contained many primary building units (TO4) as the nucleation sites in the second process of chabazite crystal reconstruction, which nucleated rapidly again under the promotion of fluorine anion. With the further prolongation of crystallization time, the regenerated secondary structural units connected together to reconstruct the framework structure of chabazite zeolite, and gradually grew into a continuous and dense membrane layer with the cross-linking growth of chabazite zeolite. In addition, chabazite zeolite membrane exhibited high permeation flux and excellent long-term hydrothermal stability for the separation of water-rich mixtures. For 50 wt% EtOH/H2O and 50 wt% IPA/H2O binary mixtures at 348 K, the stable permeation fluxes of the membranes were as high as 13.50 kg m−2 h−1 and 14.80 kg m−2 h−1, respectively.
中文翻译:
有机无模板菱沸石膜的形成过程及其对富水混合物的分离性能
详细研究了菱沸石晶种在无有机模板、含氟合成凝胶中向菱沸石分子筛膜的生长过程。表征结果表明,无有机模板菱沸石膜的形成过程包括晶种溶解过程和菱沸石晶体重构过程。在种子溶解成无定形的第一个过程中,除了少量的 4Rs 存在外,CHA 骨架的二级结构单元(D6Rs)被完全破坏。虽然无定形包含许多主要建筑单元(TO 4) 作为菱沸石晶体重建第二过程中的形核位点,在氟阴离子的促进下再次迅速形核。随着结晶时间的进一步延长,再生的二级结构单元连接在一起,重构了菱沸石的骨架结构,并随着菱沸石的交联生长逐渐成长为连续致密的膜层。此外,菱沸石分子筛膜在富水混合物的分离中表现出高渗透通量和优异的长期水热稳定性。对于 348 K 的 50 wt% EtOH/H 2 O 和 50 wt% IPA/H 2 O 二元混合物,膜的稳定渗透通量高达 13.50 kg m -2 h -1和 14.80 kg m -2 h -1,分别。