Selective ion transport through hydrated micropores in polymer membranes

Wang, Anqi; Breakwell, Charlotte; Foglia, Fabrizia; Tan, Rui; Lovell, Louie; Wei, Xiaochu; Wong, Toby; Meng, Naiqi; Li, Haodong; Seel, Andrew; Sarter, Mona; Smith, Keenan; Alvarez‐Fernandez, Alberto; Furedi, Mate; Guldin, Stefan; Britton, Melanie M.; McKeown, Neil B.; Jelfs, Kim E.; Song, Qilei

doi:10.1038/s41586-024-08140-2

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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

, Qilei Song

Nature, Volume: 635, Issue: 8038, Pages: 353 - 358

Swansea University Author: Rui Tan

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DOI (Published version): 10.1038/s41586-024-08140-2

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....

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Published in:	Nature
ISSN:	0028-0836 1476-4687
Published:	Springer Science and Business Media LLC 2024
Online Access:	Check full text
URI:	https://cronfa.swan.ac.uk/Record/cronfa68345

first_indexed	2024-11-26T19:47:27Z
last_indexed	2025-01-13T20:34:20Z
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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.</abstract><type>Journal Article</type><journal>Nature</journal><volume>635</volume><journalNumber>8038</journalNumber><paginationStart>353</paginationStart><paginationEnd>358</paginationEnd><publisher>Springer Science and Business Media LLC</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>0028-0836</issnPrint><issnElectronic>1476-4687</issnElectronic><keywords/><publishedDay>14</publishedDay><publishedMonth>11</publishedMonth><publishedYear>2024</publishedYear><publishedDate>2024-11-14</publishedDate><doi>10.1038/s41586-024-08140-2</doi><url/><notes/><college>COLLEGE NANME</college><department>Engineering and Applied Sciences School</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>EAAS</DepartmentCode><institution>Swansea University</institution><apcterm>Another institution paid the OA fee</apcterm><funders>This work was funded by the European Research Council under the European Union’s Horizon 2020 research and innovation programme (ERC-StG-PE8-NanoMMES number 851272, CoMMaD number 758370), the Engineering and Physical Sciences Research Council (EPSRC, EP/V047078/1, EP/W033356/1, EP/V057863/1, EP/W033321/1 and EP/K039245/1), the UK Research and Innovation (UKRI) Impact Acceleration Account (EP/X52556X/1) and UKRI under the UK Government’s Horizon Europe funding guarantee (EP/Y014391/1). C.B. acknowledges an EPSRC iCASE PhD studentship funded by EPSRC and Shell. T.W. acknowledges an EPSRC CDT PhD studentship funded by EPSRC and bp-ICAM. We thank D. Liu for help with atomic force microscopy; P. A. A. Klusener for industrial insights; and Z. Jiang for providing PAN support membranes and discussions. We also thank Surface Measurement Systems for help with DVS measurements, the neutron scattering facilities at ISIS (Didcot, UK) for the award of beamtime necessary to carry out these experiments, and N. C. Osti at SNS for help with beamline support. Work at Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. 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spelling	2025-01-13T15:39:07.1206717 v2 68345 2024-11-26 Selective ion transport through hydrated micropores in polymer membranes 774c33a0a76a9152ca86a156b5ae26ff 0009-0001-9278-7327 Rui Tan Rui Tan true false 2024-11-26 EAAS 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. Journal Article Nature 635 8038 353 358 Springer Science and Business Media LLC 0028-0836 1476-4687 14 11 2024 2024-11-14 10.1038/s41586-024-08140-2 COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University Another institution paid the OA fee This work was funded by the European Research Council under the European Union’s Horizon 2020 research and innovation programme (ERC-StG-PE8-NanoMMES number 851272, CoMMaD number 758370), the Engineering and Physical Sciences Research Council (EPSRC, EP/V047078/1, EP/W033356/1, EP/V057863/1, EP/W033321/1 and EP/K039245/1), the UK Research and Innovation (UKRI) Impact Acceleration Account (EP/X52556X/1) and UKRI under the UK Government’s Horizon Europe funding guarantee (EP/Y014391/1). C.B. acknowledges an EPSRC iCASE PhD studentship funded by EPSRC and Shell. T.W. acknowledges an EPSRC CDT PhD studentship funded by EPSRC and bp-ICAM. We thank D. Liu for help with atomic force microscopy; P. A. A. Klusener for industrial insights; and Z. Jiang for providing PAN support membranes and discussions. We also thank Surface Measurement Systems for help with DVS measurements, the neutron scattering facilities at ISIS (Didcot, UK) for the award of beamtime necessary to carry out these experiments, and N. C. Osti at SNS for help with beamline support. Work at Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. ORNL is managed by UT-Battelle, LLC, for US DOE under contract number DEAC05-00OR22725. 2025-01-13T15:39:07.1206717 2024-11-26T14:57:10.1721265 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Anqi Wang 0000-0003-3409-823x 1 Charlotte Breakwell 2 Fabrizia Foglia 0000-0002-2847-3489 3 Rui Tan 0009-0001-9278-7327 4 Louie Lovell 0009-0009-0045-0101 5 Xiaochu Wei 0009-0002-8945-9311 6 Toby Wong 7 Naiqi Meng 0009-0008-9310-228x 8 Haodong Li 9 Andrew Seel 10 Mona Sarter 0000-0003-1867-5543 11 Keenan Smith 12 Alberto Alvarez‐Fernandez 13 Mate Furedi 0000-0002-4300-0591 14 Stefan Guldin 0000-0002-4413-5527 15 Melanie M. Britton 0000-0003-3808-1590 16 Neil B. McKeown 0000-0002-6027-261x 17 Kim E. Jelfs 0000-0001-7683-7630 18 Qilei Song 0000-0001-8570-3626 19
title	Selective ion transport through hydrated micropores in polymer membranes
spellingShingle	Selective ion transport through hydrated micropores in polymer membranes Rui Tan
title_short	Selective ion transport through hydrated micropores in polymer membranes
title_full	Selective ion transport through hydrated micropores in polymer membranes
title_fullStr	Selective ion transport through hydrated micropores in polymer membranes
title_full_unstemmed	Selective ion transport through hydrated micropores in polymer membranes
title_sort	Selective ion transport through hydrated micropores in polymer membranes
author_id_str_mv	774c33a0a76a9152ca86a156b5ae26ff
author_id_fullname_str_mv	774c33a0a76a9152ca86a156b5ae26ff_***_Rui Tan
author	Rui Tan
author2	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 Qilei Song
format	Journal article
container_title	Nature
container_volume	635
container_issue	8038
container_start_page	353
publishDate	2024
institution	Swansea University
issn	0028-0836 1476-4687
doi_str_mv	10.1038/s41586-024-08140-2
publisher	Springer Science and Business Media LLC
college_str	Faculty of Science and Engineering
hierarchytype
hierarchy_top_id	facultyofscienceandengineering
hierarchy_top_title	Faculty of Science and Engineering
hierarchy_parent_id	facultyofscienceandengineering
hierarchy_parent_title	Faculty of Science and Engineering
department_str	School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
document_store_str	0
active_str	0
description	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.
published_date	2024-11-14T05:41:06Z
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score	11.04748

Selective ion transport through hydrated micropores in polymer membranes

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