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Cited by 115Electrostatics and Colloid InteractionsPolymer Surface Interaction StudiesAdvanced Polymer Synthesis and Characterization

Structure of Polyelectrolyte Brushes in the Presence of Multivalent Counterions

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Yu, Jing, Mao, Jun, Yuan, Guangcui, Satija, Sushil, Jiang, Zhang, Chen, Wei, Tirrell, Matthew·2016·Macromolecules
DOI 10.1021/acs.macromol.6b01064
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Abstract

Polyelectrolyte brushes are of great importance to a wide range of fields, ranging from colloidal stabilization to responsive and tunable materials to lubrication. We synthesized high-density polystyrenesulfonate (PSS) brushes using surface initiated atom transfer radical polymerization and performed neutron reflectivity (NR) and surface force measurements using a surface forces apparatus (SFA) to investigate the effect of monovalent Na +, divalent Ca 2+, Mg 2+, and Ba 2+, and trivalent Y 3+ counterions on the structure of the PSS brushes. NR and SFA results demonstrate that in monovalent salt solution the behavior of the PSS brushes agrees with scaling theory well, exhibiting two distinct regimes: the osmotic and salted brush regimes. Introducing trivalent Y 3+ cations causes an abrupt shrinkage of the PSS brush due to the uptake of Y 3+ counterions. The uptake of Y 3+ counterions and shrinkage of the brush are reversible upon increasing the concentration of monovalent salt. Divalent cations, Mg 2+, Ca 2+, and Ba 2+, while all significantly affecting the structure of PSS brushes, show strong ion specific effects that are related to the specific interactions between the divalent cations and the sulfonate groups. Our results demonstrate that the presence of multivalent counterions, even at relatively low concentrations, can strongly affect the structure of polyelectrolyte brushes. The results also highlight the importance of ion specificity to the structure of polyelectrolyte brushes in solution.

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Authors
Yu, J., Mao, J., Yuan, G., Satija, S., Jiang, Z., Chen, W., & Tirrell, M.
Affiliations
  • University of Chicago (US)
  • University of Akron (US)
  • National Institute of Standards and Technology (US)
Corresponding author
  • Chen, Wei
  • Tirrell, Matthew
ORCID
Venue
Macromolecules
Publisher
American Chemical Society (ACS)
Published
2016-07-20
Volume
49
Issue
15
Pages
5609-5617
ISSN
  • 0024-9297 (ISSN-L)
  • 1520-5835
DOI
10.1021/acs.macromol.6b01064
OpenAlex
W2493324683
Cited by
115
References
52
Citations by year
2026: 8 · 2025: 13 · 2024: 10 · 2023: 8 · 2022: 10 · 2021: 10 · 2020: 11 · 2019: 10 · 2018: 16 · 2017: 14 · 2016: 5
FWCI
10.26
Type
journal article
Language
en
Open access
Locations
  • Macromolecules (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders
Basic Energy Sciences
Topics
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Electrostatics and Colloid Interactions
  • Physical Sciences › Materials Science › Surfaces, Coatings and Films › Polymer Surface Interaction Studies
  • Physical Sciences › Chemistry › Organic Chemistry › Advanced Polymer Synthesis and Characterization
Keywords
polyelectrolyte brushes, polystyrene sulfonate, multivalent counterions, divalent cations, ion specificity, scaling theory, surface-initiated atom transfer radical polymerization

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