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Cited by 63Electrostatics and Colloid InteractionsPolymer Surface Interaction StudiesAdvanced Physical and Chemical Molecular Interactions

Comparing Solvophobic and Multivalent Induced Collapse in Polyelectrolyte Brushes

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Jackson, Nicholas E., Brettmann, Blair K., Vishwanath, Venkatram, Tirrell, Matthew, de Pablo, Juan J.·2017·ACS Macro Letters
DOI 10.1021/acsmacrolett.6b00837
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Abstract

Coarse-grained molecular dynamics enhanced by free-energy sampling methods is used to examine the roles of solvophobicity and multivalent salts on polyelectrolyte brush collapse. Specifically, we demonstrate that while ostensibly similar, solvophobic collapsed brushes and multivalent-ion collapsed brushes exhibit distinct mechanistic and structural features. Notably, multivalent-induced heterogeneous brush collapse is observed under good solvent polymer backbone conditions, demonstrating that the mechanism of multivalent collapse is not contingent upon a solvophobic backbone. Umbrella sampling of the potential of mean-force (PMF) between two individual brush strands confirms this analysis, revealing starkly different PMFs under solvophobic and multivalent conditions, suggesting the role of multivalent “bridging” as the discriminating feature in trivalent collapse. Structurally, multivalent ions show a propensity for nucleating order within collapsed brushes, whereas poor-solvent collapsed brushes are more disordered; this difference is traced to the existence of a metastable PMF minimum for poor solvent conditions, and a global PMF minimum for trivalent systems, under experimentally relevant conditions.

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Authors
Jackson, N. E., Brettmann, B. K., Vishwanath, V., Tirrell, M., & de Pablo, J. J.
Affiliations
  • Argonne National Laboratory (US)
  • University of Chicago (US)
  • The University of Chicago , , , ,
Corresponding author
Tirrell, Matthew
ORCID
Venue
ACS Macro Letters
Publisher
American Chemical Society (ACS)
Published
2017-02-03
Volume
6
Issue
2
Pages
155-160
ISSN
2161-1653 (ISSN-L)
DOI
10.1021/acsmacrolett.6b00837
OpenAlex
W2585689905
Cited by
63
References
27
Citations by year
2026: 4 · 2025: 8 · 2024: 7 · 2023: 2 · 2022: 4 · 2021: 7 · 2020: 11 · 2019: 7 · 2018: 12 · 2017: 1
FWCI
6.24
Type
journal article
Language
en
Open access
Licence
Locations
  • ACS Macro Letters (publishedVersion)
  • PubMed (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders
  • Basic Energy Sciences
  • Argonne National Laboratory
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 › Physical and Theoretical Chemistry › Advanced Physical and Chemical Molecular Interactions
Keywords
polyelectrolyte brushes, brush collapse, solvophobicity, multivalent ions, potential of mean force, umbrella sampling, coarse-grained molecular dynamics, ion bridging, nucleation, metastable states, good and poor solvents

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