Qiu Ze-Lin, Fang Li-Feng, Shen Yu-Jie, Yu Wen-Han, Zhu Bao-Ku, Hélix-Nielsen Claus, Zhang Wenjing
Key Laboratory of Macromolecule Synthesis and Functionalization (Ministry of Education), ERC of Membrane and Water Treatment (Ministry of Education), Department of Polymer Science and Engineering, Zhejiang University, Hangzhou 310027, China.
Department of Environmental Engineering, Technical University of Denmark, Bygningstorvet 115, 2800 Kgs., Lyngby, Denmark.
ACS Nano. 2021 Apr 27;15(4):7522-7535. doi: 10.1021/acsnano.1c00936. Epub 2021 Mar 29.
Separating low/high-valent ions with sub-nanometer sizes is a crucial yet challenging task in various areas (.., within environmental, healthcare, chemical, and energy engineering). Satisfying high separation precision requires membranes with exceptionally high selectivity. One way to realize this is constructing well-designed ion-selective nanochannels in pressure-driven membranes where the separation mechanism relies on combined steric, dielectric exclusion, and Donnan effects. To this aim, charged nanochannels in polyamide (PA) membranes are created by incorporating ionic polyamidoamine (PAMAM) dendrimers interfacial polymerization. Both sub-10 nm sizes of the ionic PAMAM dendrimer molecules and their gradient distributions in the PA nanofilms contribute to the successful formation of defect-free PA nanofilms, containing both internal (intramolecular voids) and external (interfacial voids between the ionic PAMAM dendrimers and the PA matrix) nanochannels for fast transport of water molecules. The external nanochannels with tunable ionizable groups endow the PA membranes with both high low/high-valent co-ion selectivity and chemical cleaning tolerance, while the ion sieving/transport mechanism was analyzed by employing the Donnan steric pore model with dielectric exclusion.
分离亚纳米尺寸的低价/高价离子在各个领域(如环境、医疗、化学和能源工程)都是一项关键但具有挑战性的任务。要实现高分离精度,需要具有极高选择性的膜。实现这一目标的一种方法是在压力驱动膜中构建精心设计的离子选择性纳米通道,其分离机制依赖于空间位阻、介电排斥和唐南效应的综合作用。为此,通过界面聚合引入离子型聚酰胺胺(PAMAM)树枝状大分子,在聚酰胺(PA)膜中创建带电纳米通道。离子型PAMAM树枝状大分子分子的亚10纳米尺寸及其在PA纳米膜中的梯度分布,都有助于成功形成无缺陷的PA纳米膜,该膜包含内部(分子内空隙)和外部(离子型PAMAM树枝状大分子与PA基质之间的界面空隙)纳米通道,用于水分子的快速传输。具有可调节电离基团的外部纳米通道赋予PA膜高的低价/高价共离子选择性和化学清洗耐受性,同时通过采用具有介电排斥的唐南空间孔模型分析了离子筛分/传输机制。