Selective ion transport through hydrated micropores in polymer membranes

Anqi Wang (), Charlotte Breakwell, Fabrizia Foglia, Rui Tan, Louie Lovell, Xiaochu Wei, Toby Wong, Naiqi Meng, Haodong Li, Andrew Seel, Mona Sarter, Keenan Smith, Alberto Alvarez‐Fernandez, Mate Furedi, Stefan Guldin, Melanie M. Britton, Neil B. McKeown, Kim E. Jelfs and Qilei Song ()
Additional contact information
Anqi Wang: Imperial College London
Charlotte Breakwell: Imperial College London
Fabrizia Foglia: University College London
Rui Tan: Imperial College London
Louie Lovell: University of Birmingham
Xiaochu Wei: Imperial College London
Toby Wong: Imperial College London
Naiqi Meng: Imperial College London
Haodong Li: Imperial College London
Andrew Seel: Harwell Science and Innovation Campus
Mona Sarter: Harwell Science and Innovation Campus
Keenan Smith: University College London
Alberto Alvarez‐Fernandez: University College London
Mate Furedi: University College London
Stefan Guldin: University College London
Melanie M. Britton: University of Birmingham
Neil B. McKeown: University of Edinburgh
Kim E. Jelfs: Imperial College London
Qilei Song: Imperial College London

Nature, 2024, vol. 635, issue 8038, 353-358

Abstract: Abstract Ion-conducting polymer membranes are essential in many separation processes and electrochemical devices, including electrodialysis1, redox flow batteries2, fuel cells3 and electrolysers4,5. Controlling ion transport and selectivity in these membranes largely hinges on the manipulation of pore size. Although membrane pore structures can be designed in the dry state6, they are redefined upon hydration owing to swelling in electrolyte solutions. Strategies to control pore hydration and a deeper understanding of pore structure evolution are vital for accurate pore size tuning. Here we report polymer membranes containing pendant groups of varying hydrophobicity, strategically positioned near charged groups to regulate their hydration capacity and pore swelling. Modulation of the hydrated micropore size (less than two nanometres) enables direct control over water and ion transport across broad length scales, as quantified by spectroscopic and computational methods. Ion selectivity improves in hydration-restrained pores created by more hydrophobic pendant groups. These highly interconnected ion transport channels, with tuned pore gate sizes, show higher ionic conductivity and orders-of-magnitude lower permeation rates of redox-active species compared with conventional membranes, enabling stable cycling of energy-dense aqueous organic redox flow batteries. This pore size tailoring approach provides a promising avenue to membranes with precisely controlled ionic and molecular transport functions.

Date: 2024
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DOI: 10.1038/s41586-024-08140-2

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