Nano-confined controllable crystallization in supramolecular polymeric membranes for ultra-selective desalination

Gang Lu (), Hubao A, Yuanyuan Zhao, Yan Zhao, Hengyue Xu, Wentao Shang, Xi Chen, Jiawei Sun, Huacheng Zhang, Jun Wu, Bing Dai, Bart Bruggen, Raf Dewil, Alicia Kyoungjin An () and Shuang Zheng ()
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Gang Lu: City University of Hong Kong
Hubao A: Wuhan University
Yuanyuan Zhao: The Hong Kong Polytechnic University
Yan Zhao: KU Leuven
Hengyue Xu: Tsinghua University
Wentao Shang: Jinan University
Xi Chen: City University of Hong Kong
Jiawei Sun: City University of Hong Kong
Huacheng Zhang: RMIT University
Jun Wu: Harbin Engineering University
Bing Dai: Shenzhen University
Bart Bruggen: KU Leuven
Raf Dewil: KU Leuven
Alicia Kyoungjin An: City University of Hong Kong
Shuang Zheng: The University of Hong Kong

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Innovations in self-assembly and aggregate engineering have led to membranes that better balance water permeability with salt rejection, overcoming traditional trade-offs. Here we demonstrate a strategy that uses multivalent H-bond interactions at the nano-confined space to manipulate controllable and organized crystallization. Specifically, we design amphiphilic oligomers featuring hydrophobic segments with strongly polar end-capped motifs. When spreading on air/water interfaces, the hydrophobic parts repel water, yielding an ordered alignment of supramolecular oligomers under nano-confinement, while the strongly polar sections engage in strong hydrogen bonding and reconfigure to strongly interact with water molecules, enabling the controlled assembly and orientation of nano-confined crystalline domains. This arrangement provides dual benefits: refining the distribution of pore sizes for ultra-selectivity and boosting the free volume for water permeation. Compared to counterpart oligomers with weakly polar motifs, the optimized membrane with a 6-nm thickness demonstrates the water permeability of 14.8 L m−2 h−1 bar−1 and extraordinary water/NaCl selectivity of more than 54 bar−1 under pressure-driven condition. This study sheds light on how nano-confined self-assembly and aggregate engineering affect the architectures, functionality, and performance of polymer membranes, emphasizing the promise of controllable crystallization in ultrathin membranes for optimal desalination.

Date: 2025
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DOI: 10.1038/s41467-025-57353-0

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