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Insights into the Role of Counterions on Polyelectrolyte-Modified Nanopore Accessibility

Silies, Laura ; Gonzalez Solveyra, Estefania ; Szleifer, Igal ; Andrieu-Brunsen, Annette (2022):
Insights into the Role of Counterions on Polyelectrolyte-Modified Nanopore Accessibility. (Postprint)
In: Langmuir, 34 (20), ACS Publications, ISSN 0743-7463, e-ISSN 1520-5827,
DOI: 10.26083/tuprints-00021737,
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Item Type: Article
Origin: Secondary publication service
Status: Postprint
Title: Insights into the Role of Counterions on Polyelectrolyte-Modified Nanopore Accessibility
Language: English
Abstract:

Nanopores play a decisive role in different technologies from oil production, separation, and sensing to drug delivery or catalysis and energy conversion. In recent years, abilities to functionalize nanopores have advanced significantly. Thereby, nanopores functionalized with polyelectrolytes or responsive polymers show fascinating transport properties, such as gated or gradually controlled ionic permselectivity. Nonetheless, understanding the influence of external parameters such as ion type or concentration on nanopore performance, and thus on the mentioned applications, remains a challenge but is crucial for applications. In this work, the effect of different counterions on the wetting and ionic transport in poly(2-(methacryloyloxy)ethyltrimethylammonium chloride)-functionalized silica mesopores (pore diameter <10 nm) was experimentally and theoretically investigated. Static contact angles covered a range from 45 to almost 90° by exclusively changing the counterion. Ionic pore accessibility was also strongly dependent on the counterion present and was found to gradually change from accessible pores up to complete, pH-independent ion exclusion. On the basis of molecular theory calculations, these experimental observations were rationalized on the basis of ion binding between the [2-(methacryloyloxy)ethyl]trimethylammonium chloride monomers and the counterions. In addition, the theoretical framework provided a nanoscopic view into the molecular organization inside the pores, showing a strong dependence of ion concentration and ion distribution profiles along the pore radius in dependence of the present ions. The obtained insights on the role of counterion type and ion binding in nanopores are expected to have direct impact on the above-mentioned applications.

Journal or Publication Title: Langmuir
Volume of the journal: 34
Issue Number: 20
Place of Publication: Darmstadt
Publisher: ACS Publications
Collation: 27 Seiten
Uncontrolled Keywords: mesoporous silica films, polyelectrolyte, counterion, wetting, ionic permselectivity, ion binding
Classification DDC: 500 Naturwissenschaften und Mathematik > 540 Chemie
Divisions: DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres > CRC 1194: Interaction between Transport and Wetting Processes > Research Area C: New and Improved Applications > C04: Controlled Dynamic Wetting and the Influence of Ionic Mass Transport in Mesoporous Film
Profile Areas > Thermo-Fluids & Interfaces
07 Department of Chemistry > Fachgebiet Makromolekulare Chemie
Date Deposited: 21 Jul 2022 13:04
Last Modified: 11 Jan 2023 14:15
DOI: 10.26083/tuprints-00021737
Corresponding Links:
URN: urn:nbn:de:tuda-tuprints-217375
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/21737
PPN: 503518166
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