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Swelling Behavior of Composite Systems: Mutual Effects between Polyelectrolyte Brushes and Multilayers

Cite this: Macromolecules 2018, 51, 8, 2996–3005
Publication Date (Web):April 6, 2018
https://doi.org/10.1021/acs.macromol.8b00359
Copyright © 2018 American Chemical Society
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Abstract

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The combination of polyelectrolyte multilayers (PEMs) and end-grafted brushes represents a valuable approach to the design of complex organic composite materials with tailored responsive properties. This article addresses the correlation between the swelling properties of composites and their internal structure. Here, we present composites of end-grafted 2-(methacryloyloxy)ethyl-trimethylammonium chloride (PMETAC) brushes covered with poly(sodium styrenesulfonate) (PSS) and poly(diallyldimethylammonium) chloride (PDADMAC) PEMs and characterize them under various relative humidities. Ellipsometry and neutron reflectometry are carried out to monitor the swelling behavior and the internal structure, respectively, of the composites, giving evidence of a significant mutual influence of the two components. The reflectivity data reveal a deep penetration of the PEMs’ polyelectrolyte chains into the underlying brush but also a significant humidity dependence of their spatial distribution, indicating considerable mobility within the brush. In contrast to a compact bare brush, for composites a pronounced stretching of the brush after PEM adsorption is observed. The water uptake of the brush is reduced. A PEM on top of a brush is less influenced by the latter one. Swelling gradually reduces the brush/PEM interpenetration, while water accumulates in the interfacial region between the brush and PEM so that these two compartments get increasingly separated with increasing humidity. The swelling process is largely reversible, which demonstrates the potential applicability of these composites as chemical gas or moisture sensors.

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  • Full data sets, best fits, SLD profiles, and volume fraction profiles for all measurements (PDF)

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Cited By

This article is cited by 10 publications.

  1. Guido C. Ritsema van Eck, Leonardo Chiappisi, Sissi de Beer. Fundamentals and Applications of Polymer Brushes in Air. ACS Applied Polymer Materials 2022, 4 (5) , 3062-3087. https://doi.org/10.1021/acsapm.1c01615
  2. Neng Hu, Chen Chen, Ezzeldin Metwalli, Lorenz Bießmann, Christian Herold, Jun Fu, Robert Cubitt, Qi Zhong, Peter Müller-Buschbaum. Hydration and Thermal Response Kinetics of a Cross-Linked Thermoresponsive Copolymer Film on a Hydrophobic PAN Substrate Coating Probed by In Situ Neutron Reflectivity. Langmuir 2021, 37 (22) , 6819-6829. https://doi.org/10.1021/acs.langmuir.1c00931
  3. Qi Zhong, Neng Hu, Lei Mi, Ji-Ping Wang, Ezzeldin Metwalli, Lorenz Bießmann, Christian Herold, Jing Yang, Guang-Peng Wu, Zhi-Kang Xu, Robert Cubitt, Peter Müller-Buschbaum. Impact of Thermal History on the Kinetic Response of Thermoresponsive Poly(diethylene glycol monomethyl ether methacrylate)-block-poly(poly(ethylene glycol)methyl ether methacrylate) Thin Films Investigated by In Situ Neutron Reflectivity. Langmuir 2020, 36 (22) , 6228-6237. https://doi.org/10.1021/acs.langmuir.0c00866
  4. Mihaela Delcea, Christiane A. Helm. X-ray and Neutron Reflectometry of Thin Films at Liquid Interfaces. Langmuir 2019, 35 (26) , 8519-8530. https://doi.org/10.1021/acs.langmuir.8b04315
  5. Max Wolff, Henrich Frielinghaus, Marité Cárdenas, Juan Fransisco Gonzalez, Katharina Theis-Bröhl, Olaf Softwedel, Regine von Klitzing, Georgia A. Pilkington, Mark W. Rutland, Reiner Dahint, Philipp Gutfreund. Grazing incidence neutron scattering for the study of solid–liquid interfaces. 2023,,https://doi.org/10.1016/B978-0-323-85669-0.00014-3
  6. Xu Jia, Jiao Xie, Xinhua Zhan, Xuedong Gong, Yuejun Zhang. Thermal decomposition mechanism of poly(dimethyldiallylammonium chloride). Journal of Thermal Analysis and Calorimetry 2022, 147 (7) , 4589-4596. https://doi.org/10.1007/s10973-021-10860-w
  7. Xingqin Fu, Yuejun Zhang, Xu Jia, Yongji Wang, Tingting Chen. Research Progress on Typical Quaternary Ammonium Salt Polymers. Molecules 2022, 27 (4) , 1267. https://doi.org/10.3390/molecules27041267
  8. Da Zhang, Qing‐Shuang Li, Zi‐Xuan Liang, Xia‐Chao Chen, Junran Hao, Juming Yao, Chun‐Xin Lu, Yahong Zhou, Lei Jiang. Laser‐Directed Foaming of Hydroplastic Polyelectrolyte Films toward Tunable Structures and Programmable Routes. Advanced Functional Materials 2022, 32 (8) , 2107598. https://doi.org/10.1002/adfm.202107598
  9. Samantha Micciulla, Dominic W. Hayward, Yuri Gerelli, Alain Panzarella, Regine von Klitzing, Michael Gradzielski, Leonardo Chiappisi. One-step procedure for the preparation of functional polysaccharide/fatty acid multilayered coatings. Communications Chemistry 2019, 2 (1) https://doi.org/10.1038/s42004-019-0155-y
  10. Dikran Boyaciyan, Larissa Braun, Oliver Löhmann, Luca Silvi, Emanuel Schneck, Regine von Klitzing. Gold nanoparticle distribution in polyelectrolyte brushes loaded at different pH conditions. The Journal of Chemical Physics 2018, 149 (16) , 163322. https://doi.org/10.1063/1.5035554

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