Continuous Covalent Organic Framework Membranes with Ordered Nanochannels as Tunable Transport Layers for Fast Butanol/Water Separation.

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-09-18 Epub Date: 2024-09-06 DOI:10.1021/acs.nanolett.4c02458

Hukang Guo, Yijie Fang, Jiaqi Li, Weilin Feng, Chuanjie Fang, Liping Zhu

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Abstract

Polymeric membranes with high permselective performance are desirable for energy-saving bioalcohol separations. However, it remains challenging to design membrane microstructures with low-resistance channels and a thin thickness for fast alcohol transport. Herein, we demonstrate highly crystalline covalent organic framework (COF) membranes with ordered nanochannels as tunable transport layers for efficient butanol/water separation. The thickness was well-regulated by altering the concentration and molar ratio of two aldehyde monomers with different reactivity. The surface-integrated poly(dimethylsiloxane) produced defect-free and hydrophobic COF membranes. The membrane with continuous transport channels exhibited an exceptional flux of up to 18.8 kg m^-2 h^-1 and a pervaporation separation index of 217.7 kg m^-2 h^-1 for separating 5 wt % n-butanol/water. The separation efficiency exceeded that of analogous membranes. The calculated mass-transfer coefficient of butanol followed an inverse relationship with the COF membrane thickness. Consequently, this work reveals the great potential of crystalline polymeric membranes with high-density nanopores for biofuel recovery.

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具有有序纳米通道的连续共价有机框架膜是用于快速分离丁醇/水的可调传输层。

对于节能型生物酒精分离而言，具有高过选择性的聚合物膜是理想之选。然而，设计具有低阻力通道和薄厚度的膜微结构以实现酒精的快速传输仍具有挑战性。在此，我们展示了具有有序纳米通道的高结晶共价有机框架（COF）膜，可作为高效丁醇/水分离的可调传输层。通过改变两种具有不同反应活性的醛单体的浓度和摩尔比，可以很好地调节膜的厚度。表面集成聚（二甲基硅氧烷）产生了无缺陷和疏水的 COF 膜。在分离 5 wt % 正丁醇/水时，带有连续传输通道的膜表现出了高达 18.8 kg m-2 h-1 的超常通量和 217.7 kg m-2 h-1 的渗透分离指数。分离效率超过了同类膜。计算得出的丁醇传质系数与 COF 膜厚度呈反比关系。因此，这项研究揭示了具有高密度纳米孔的结晶聚合物膜在生物燃料回收方面的巨大潜力。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.