Insights into the Enhancement of MOF/Polymer Adhesion in Mixed-Matrix Membranes via Polymer Functionalization
Insights into the Enhancement of MOF/Polymer Adhesion in Mixed-Matrix Membranes via Polymer Functionalization
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DOI：
10.1021/acsami.1c03859
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发表时间：
2021-06-09
影响因子：
9.5
通讯作者：
Maurin, Guillaume
中科院分区：
文献类型：
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作者：
Carja, Ionela-Daniela;Tavares, Sergio Rodrigues;Maurin, Guillaume
使用标准路线制备的基于M0 F的混合基质膜（MMM）通常在聚合物和M0 F之间表现出差的粘附性。在这里，我们报告了一个前所未有的系统探索聚合物功能化的关键，实现无缺陷的金属记忆合金。作为一个案例研究，我们探索了计算MMM的基础上的原型U10 -66（锆）MOF与聚合物的固有孔隙度-1（PIM-1）功能化的各种基团，包括偕胺肟，四唑，和N-（（2-乙醇氨基）乙基）甲酰胺的组合。明显地，预测偕胺肟衍生物PIM-1/U10 -66（Zr）MMM表达所需的增强的MOF/聚合物界面相互作用，因此随后进行制备和实验评估。显著地，高分辨率透射电子显微镜证实了两种组分之间的最佳粘附，与原始PIM-1/UiO-66（Zr）MMM所示的纳米尺寸的空隙/缺陷形成对比。值得注意的是，单一气体渗透测量进一步证实了最佳MOF/聚合物粘附的需要，以便有效地使MOF能够在所得MMM的气体输送中发挥作用。
MOF-based mixed-matrix membranes (MMMs) prepared using standard routes often exhibit poor adhesion between polymers and MOFs. Herein, we report an unprecedented systematic exploration on polymer functionalization as the key to achieving defect-free MMMs. As a case study, we explored computationally MMMs based on the combination of the prototypical UiO-66(Zr) MOF with polymer of intrinsic porosity-1 (PIM-1) functionalized with various groups including amidoxime, tetrazole, and N-((2-ethanolamino)ethyl)carboxamide. Distinctly, the amidoxime-derivative PIM-1/UiO-66(Zr) MMM was predicted to express the desired enhanced MOF/polymer interfacial interactions and thus subsequently prepared and evaluated experimentally. Prominently, high-resolution transmission electron microscopy confirmed optimal adhesion between the two components in contrast to the nanometer-sized voids/defects shown by the pristine PIM-1/UiO-66(Zr) MMM. Notably, single-gas permeation measurements further corroborated the need of optimal MOF/polymer adhesion in order to effectively enable the MOF to play a role in the gas transport of the resulting MMM.