Effect of Thickness on the pH Responsiveness of Strong Polyelectrolyte Brushes

Guang-Tao Mei; Yue Huang; Jian Zhang; Guang-Ming Liu

doi:10.1007/s10118-025-3464-x

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Effect of Thickness on the pH Responsiveness of Strong Polyelectrolyte Brushes

RAPID COMMUNICATION | Updated：2025-12-03

- Effect of Thickness on the pH Responsiveness of Strong Polyelectrolyte Brushes
- Effect of Thickness on the pH Responsiveness of Strong Polyelectrolyte Brushes
- Chinese Journal of Polymer Science 2025年43卷第12期页码：2185-2190
- Affiliations：
  
  a.Hefei National Research Center for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China
  b.Zhejiang Key Laboratory of Bio-based Health Functional Fiber Materials, College of Material and Textile Engineering, Jiaxing University, Jiaxing 314001, China
- Author bio：
  
  jz09275@zjxu.edu.cn (J.Z.)
  gml@ustc.edu.cn (G.M.L.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 22273098, 52033001 and 22303032), the Key Project of Anhui Province Science and Technology Innovation Platform (No. S202305a12020030), and the Science and Technology Program Project of Zhejiang Province, China (No. 2025ZY01057). This work was partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication.;Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-025-3464-x.
- DOI：10.1007/s10118-025-3464-x
  中图分类号：
- 收稿：2025-07-16，
  
  录用：2025-09-27，
  
  网络首发：2025-11-19，
  
  纸质出版：2025-12-15
- Accepted：
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Mei, G. T.; Huang, Y.; Zhang, J.; Liu, G. M. Effect of thickness on the pH responsiveness of strong polyelectrolyte brushes. Chinese J. Polym. Sci. 2025, 43, 2185–2190

Guang-Tao Mei, Yue Huang, Jian Zhang, et al. Effect of Thickness on the pH Responsiveness of Strong Polyelectrolyte Brushes[J]. Chinese Journal of Polymer Science, 2025, 43(12): 2185-2190.
Mei, G. T.; Huang, Y.; Zhang, J.; Liu, G. M. Effect of thickness on the pH responsiveness of strong polyelectrolyte brushes. Chinese J. Polym. Sci. 2025, 43, 2185–2190 DOI： 10.1007/s10118-025-3464-x.

Guang-Tao Mei, Yue Huang, Jian Zhang, et al. Effect of Thickness on the pH Responsiveness of Strong Polyelectrolyte Brushes[J]. Chinese Journal of Polymer Science, 2025, 43(12): 2185-2190. DOI： 10.1007/s10118-025-3464-x.

摘要

For strong polyelectrolyte brushes

the pH-responsive hydration and stiffness are dependent on brush thickness

and the pH-responsive adhesion and wettability are independent of brush thickness.

Abstract

Strong polyelectrolyte brushes (SPBs) play an important role in enabling material surface functionalization due to their unique stimuli-responsive properties. Although the unexpected pH responsiveness of SPBs has been revealed in the past ten years

it is still unclear if the pH-responsive properties of SPBs are affected by the brush thickness. In this study

we employed the positively charged poly[2-(methacryloyloxy)ethyl] trimethylammonium chloride (PMETAC) and negatively charged sodium poly(styrenesulfonate) (NaPSS) brushes as model systems to explore the effect of thickness on the pH-responsive properties of SPBs. The results demonstrate that the pH-responsive properties of SPBs manifest different dependences on the brush thickness. Specifically

for both PMETAC and NaPSS brushes

the pH-responsive hydration and stiffness are influenced by the thickness

and the pH-responsive wettability and adhesion are almost unaffected by the thickness. This work not only provides a clear understanding of the relationship between the brush thickness and the pH responsiveness of SPBs

but also offers a new method to control the pH-responsive properties of SPBs.

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references

[Ren, H.; Qiu, X. P.; Shi, Y.; Yang, P.; Winnik, F. M. pH-dependent morphology and photoresponse of azopyridine-terminated poly(N-isopropylacrylamide) nanoparticles in Water. Macromolecules 2019, 52 , 2939-2948..

Ren, H.; Qiu, X. P.; Shi, Y.; Yang, P.; Winnik, F. M. The two phase transitions of hydrophobically end-capped poly(N-isopropylacrylamide)s in water. Macromolecules 2020 , 53 , 5105−5115..

Ren, H.; Qiu, X. P.; Shi, Y.; Yang, P.; Winnik, F. M. Light, temperature, and pH control of aqueous azopyridine-terminated poly(N-isopropylacrylamide) solutions. Polym. Chem. 2019 , 10 , 5080−5086..

Ren, H.; Yang, P.; Winnik, F. M. Azopyridine: a smart photo- and chemo-responsive substituent for polymers and supramolecular assemblies. Polym. Chem. 2020 , 11 , 5955−5961..

Shi, Y.; Peng, H.; Yang, J. F.; Zhao, J. Counterion binding dynamics of a polyelectrolyte. Macromolecules 2021 , 54 , 4926−4933..

Muthukumar, M. A perspective on polyelectrolyte solutions. Macromolecules 2017 , 50 , 9528−9560..

Shen, Y.; Le, X.; Wu, Y.; Chen, T. Stimulus-responsive polymer materials toward multi-mode and multi-level information anti-counterfeiting: recent advances and future challenges. Chem. Soc. Rev. 2024 , 53 , 606−623..

Ren, H.; Chen, H.; Kang, Y.; Liu, W.; Liu, Y. C.; Tao, F.; Miao, S. T.; Zhang, Y. Y.; Liu, Q.; Dong, M. D.; Liu, Y. G.; Liu, B.; Yang, P. Non-fibril amyloid aggregation at the air/water interface: self-adaptive pathway resulting in a 2D janus nanofilm. Chem. Sci. 2024 , 15 , 8946−8958..

Bai, J. W.; Liu, W.; Wen, B.; Lei, Z. L.; Li, C.; Ren, H.; Yang, P. Synergistic functional group interactions for stable interfacial adhesion: insights from amyloid-inspired polymers. Chinese J. Polym. Sci. 2025 , 43 , 1096−1104..

Smook, L. A.; Dahlin, A.; Schroën, K.; de Beer, S. Responsive polyelectrolyte brushes in applications: functions, stimuli, and design considerations. Adv. Mater. 2025 , 37 , e09580..

Wu, J.; Hua, Z.; Liu, G. Supramolecular adhesives inspired from adhesive proteins and nucleic acids: molecular design, properties, and applications. Soft Matter 2025 , 21 , 324−341..

Dong, Z.; Wu, J.; Shen, X. Y.; Hua, Z.; Liu, G. M. Bioinspired nucleobase-contain ing polyelectrolytes as robust and tunable adhesives by balancing the adhesive and cohesive properties. Chem. Sci. 2023 , 14 , 3938−3948..

Xiong, T. Y.; Li, C. W.; He, X. L.; Xie, B. Y.; Zong, J. W.; Jiang, Y. A.; Ma, W. J.; Wu, F.; Fei, J. J.; Yu, P.; Mao, L. Q. Neuromorphic functions with a polyelectrolyte-confined fluidic memristor. Science 2023 , 379 , 156−161..

Yu, J.; Jackson, N. E.; Xu, X.; Morgenstern, Y.; Kaufman, Y.; Ruths, M.; de Pablo, J. J.; Tirrell, M. Multivalent counterions diminish the lubricity of polyelectrolyte brushes. Science 2018 , 360 , 1434−1438..

He, Z. Y.; Xie, W. J.; Liu, Z. Q.; Liu, G. M.; Wang, Z. W.; Gao, Y. Q.; Wang, J. J. Tuning ice nucleation with counterions on polyelectrolyte brush surfaces. Sci. Adv. 2016 , 2 , e1600345..

Dai,L. H.; Xu, F.; Huang, K.; Xia, Y. S.; Wang, Y. X.; Qu, K.; Xin, L.; Zhang, D. Z.; Xiong, Z. D.; Wu, Y. L.; Guo, X. H.; Jin, W. Q.; Xu, Z. Ultrafast water transport in two-dimensional channels enabled by spherical polyelectrolyte brushes with controllable flexibility. Angew. Chem. Int. Ed. 2021 , 60 , 19933−19941..

He, X. L.; Zhang, K. L.; Li, T.; Jiang, Y. N.; Yu, P.; Mao, L. Q. Micrometer-scale ion current rectification at polyelectrolyte brush-modified micropipets. J. Am. Chem. Soc. 2017 , 139 , 1396−1399..

Wang, J.; Hu, F.; Sant, S.; Chu, K.; Riemer, L.; Damjanovic, D.; Kilbey II, S. M.; Klok, H. A. Pyroelectric polyelectrolyte brushes. Adv. Mater. 2024 , 36 , 2307038..

Chernyy, S.; Järn, M.; Shimizu, K.; Swerin, A.; Pedersen, S. U.; Daasbjerg, K.; Makkonen, L.; Claesson, P.; Iruthayaraj, J. Superhydrophilic polyelectrolyte brush layers with imparted anti-icing properties: effect of counter ions. ACS Appl. Mater. Interfaces 2014 , 6 , 6487−6496..

Huang, Y.; Mei, G. T.; Hua, Z.; Liu, G. M. Counterion-mediated hydrogen bonding making strong polyelectrolytes pH-responsive: current understanding and perspectives. Chinese J. Polym. Sci. 2024 , 42 , 1270−1277..

Zhang, J.; Kou, R.; Liu, G. M. Effect of salt concentration on the pH responses of strong and weak polyelectrolyte brushes. Langmuir 2017 , 33 , 6838−6845..

Topham, P. D.; Glidle, A.; Toolan, D. T. W.; Weir, M. P.; Skoda, M. W. A.; Barker, R.; Howse, J. R. The relationship between charge density and polyelectrolyte brush profile using simultaneous neutron reflectivity and in situ attenuated total internal reflection FTIR. Langmuir 2013 , 29 , 6068−6076..

Geoghegan, M. Weak polyelectrolyte brushes. Soft Matter 2022 , 18 , 2500−2511..

Zhang, J.; Hua, Z.; Liu, G. M. Effect of counterion-mediated hydrogen bonding on polyelectrolytes at the solid/water interface: current understanding and perspectives. Langmuir 2023 , 39 , 2881−2889..

Wu, B.; Wang, X. W.; Yang, J.; Hua, Z.; Tian, K. Z.; Kou, R.; Zhang, J.; Ye, S. J.; Luo, Y.; Craig, V. S. J.; Zhang, G. Z.; Liu, G. M. Reorganization of hydrogen bond network makes strong polyelectrolyte brushes pH-responsive. Sci. Adv. 2016 , 2 , e1600579..

Huang, Y.; Zheng, X. X.; Ye, S. J.; Hua, Z.; Liu, G. M. Counterion-mediated hydrogen bonding making poly(styrenesulfonate)-based strong polyelectrolytes pH-responsive. J. Am. Chem. Soc. 2023 , 145 , 20745−20748..

Schüwer, N.; Klok, H.-A. Tuning the pH sensitivity of poly(methacrylic acid) brushes. Langmuir 2011 , 27 , 4789−4796..

Yadav, V.; Jannes-Lizcano, Y. A.; Dewangan, N. K.; Park, N.; Li, T. H.; Robertson, M. L.; Conrad, J. C. Tuning bacterial attachment and detachment via the thickness and dispersity of a pH-responsive polymer brush. ACS Appl. Mater. Interfaces 2017 , 9 , 44900−44910..

Zhang, H. N.; Rühe, J. Polyelectrolyte multilayers on weak polyelectrolyte brushes. Macromol. Rapid Commun. 2003 , 24 , 576−579..

Zhang, H. N.; Rühe, J. Interaction of strong polyelectrolytes with surface-attached polyelectrolyte brushes-polymer brushes as substrates for the layer-by-layer deposition of polyelectrolytes. Macromolecules 2003 , 36 , 6593−6598..

Zhang, H. N.; Rühe, J. Weak polyelectrolyte brushes as substrates for the formation of surface-attached polyelectrolyte-polyelectrolyte complexes and polyelectrolyte multilayers. Macromolecules 2005 , 38 , 10743−10749..

Xu, G. F.; Yang, J. F.; Zhao, J. Molecular weight dependence of chain conformation of strong polyelectrolytes. J. Chem. Phys. 2018 , 149 , 163329..

Jia, P.; Yang, Q.; Gong, Y.; Zhao, J. Dynamic exchange of counterions of polystyrene sulfonate. J. Chem. Phys. 2012 , 136 , 084904..

Muthukumar, M. Theory of counter-ion condensation on flexible polyelectrolytes: adsorption mechanism. J. Chem. Phys. 2004 , 120 , 9343−9350..

Manning, G. S. Limiting laws and counterion condensation in polyelectrolyte solutions.I. colligative properties. J. Chem. Phys. 1969 , 51 , 924−933..

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