唐南效应设计的共价有机骨架膜用于基于尺寸和电荷的精确分子筛分,ACS Applied Materials & Interfaces

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唐南效应设计的共价有机骨架膜用于基于尺寸和电荷的精确分子筛分
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-03 , DOI: 10.1021/acsami.3c02556
Yi-Xing Sun ₁ , Jing Zhao ₂ , Xin-Zheng Li ₃ , Han Jiang ₃ , Ya-Juan Cai ₄ , Xu Yang ₂ , Yang Liu ₁ , Yi-Bo Li ₁ , Zi-Hao Yang ₁ , Ya-Ge Wu ₁ , Li-Ye Chen ₁ , Jing-Gang Gai ₁

Affiliation

共价有机框架 (COF) 具有有序的孔隙和明确的拓扑结构，是纳滤 (NF) 膜的理想材料，因为它们具有超越渗透/选择性权衡困境的能力。然而，大多数报道的基于 COF 的膜都专注于分离不同大小的分子，导致对具有不同电荷的相似分子的选择性较低。在这里，带负电荷的 COF 层是在微孔载体上原位制造的，用于分离具有不同大小和电荷的分子。超高透水性 (216.56 L m ^–2 h ^–1 bar ^–1) 是由于有序的孔隙和优异的亲水性而获得的，这超过了大多数具有类似排斥率的膜。我们首次使用具有不同尺寸和电荷的多种染料来研究由唐南效应和尺寸排阻引起的选择性行为。获得的膜对大于 1.3 nm 的带负电和中性电荷的染料表现出优异的排斥，而尺寸为 1.6 nm 的带正电的染料可以通过膜，从而分离具有相似分子大小的负/正混合染料。这种在纳米多孔材料中结合唐南效应和尺寸排阻的策略可能会演变成用于复杂分离的通用平台。

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Donnan Effect-Engineered Covalent Organic Framework Membranes toward Size- and Charge-Based Precise Molecular Sieving

Covalent organic frameworks (COFs), with ordered pores and well-defined topology, are ideal materials for nanofiltration (NF) membranes because of their capacity of transcending the permeance/selectivity trade-off predicament. However, most reported COF-based membranes are focused on separating molecules with different sizes, resulting in low selectivity to similar molecules with different charges. Here, the negatively charged COF layer was fabricated in situ on a microporous support for the separation of molecules with different sizes and charges. Ultrahigh water permeance (216.56 L m^–2 h^–1 bar^–1) was obtained because of the ordered pores and excellent hydrophilicity, which exceeds that of most membranes with similar rejections. For the first time, we used multifarious dyes with different sizes and charges, for the investigation of the selectivity behavior caused by the Donnan effect and size exclusion. The obtained membranes represent superior rejections to negatively and neutrally charged dyes larger than 1.3 nm, while positively charged dyes with a size of 1.6 nm can pass through the membrane, resulting in the separation of negative/positive mixed dyes with similar molecular sizes. This strategy of combining the Donnan effect and size exclusion in nanoporous materials may evolve into a generic platform for sophisticated separation.

更新日期：2023-04-03

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