Jiao Chengli, Song Xiangju, Zhang Xiaoqian, Sun Lixian, Jiang Heqing
CAS Key Laboratory of Biobased Materials, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, P. R. China.
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, P. R. China.
ACS Appl Mater Interfaces. 2021 Apr 21;13(15):18380-18388. doi: 10.1021/acsami.1c03737. Epub 2021 Apr 12.
Control of the surface morphology of polyamide membranes fabricated by interfacial polymerization is of great importance in dictating the separation performance. Herein, polyamide membranes with a specific nanoscale striped Turing structure are generated through facile addition of Zr-based metal-organic framework UiO-66-NH in the aqueous triethylenetetramine phase. Interestingly, accompanied by the degradation of UiO-66-NH in aqueous solution, an intermediate complex is in situ formed through the strong interaction between the Zr metal center and the amine group from triethylenetetramine, which can lower amine diffusion and induce a local interfacial reaction, contributing to the generation of a homogeneous nanoscale striped Turing structure. The resulting membranes are used for CO/CH gas separation. Compared with the parent polyamide membrane displaying a CO/CH selectivity of 43.1 and a CO permeance of 31.5 GPU, the membrane with 0.02 wt % of UiO-66-NH introduced into the aqueous phase shows a higher CO/CH selectivity of 58.3, along with a CO permeance of 27.1 GPU. Additionally, when 0.1 wt % of UiO-66-NH is incorporated into the aqueous phase, the membrane exhibits a combination of a higher CO/CH selectivity and an enhanced CO permeance in contrast with the parent polyamide membrane.
通过界面聚合制备的聚酰胺膜的表面形态控制对于决定分离性能至关重要。在此,通过在三乙烯四胺水相中轻松添加锆基金属有机框架UiO-66-NH,生成了具有特定纳米级条纹图灵结构的聚酰胺膜。有趣的是,伴随着UiO-66-NH在水溶液中的降解,通过锆金属中心与三乙烯四胺中的胺基之间的强相互作用原位形成了一种中间络合物,它可以降低胺的扩散并引发局部界面反应,有助于生成均匀的纳米级条纹图灵结构。所得的膜用于CO/CH气体分离。与显示CO/CH选择性为43.1且CO渗透率为31.5 GPU的母体聚酰胺膜相比,在水相中引入0.02 wt% UiO-66-NH的膜显示出更高的CO/CH选择性58.3,同时CO渗透率为27.1 GPU。此外,当在水相中加入0.1 wt%的UiO-66-NH时,与母体聚酰胺膜相比,该膜表现出更高的CO/CH选择性和增强的CO渗透率的组合。