Multivalent counterions diminish the lubricity of polyelectrolyte brushes
Open accessAbstract
Polyelectrolyte brushes provide wear protection and lubrication in many technical, medical, physiological and biological applications. Wear resistance and low friction are attributed to counterion osmotic pressure and the hydration layer surrounding the charged polymer segments. However, the presence of multivalent counterions in solution can strongly affect the interchain interactions and structural properties of brush layers. We evaluated the lubrication properties of polystyrene sulfonate brush layers sliding against each other in aqueous solutions containing increasing concentrations of counterions. The presence of multivalent ions (Y3+, Ca2+, Ba2+), even at minute concentrations, dramatically increases the friction forces between brush layers due to electrostatic bridging and brush collapse. Our results suggest the lubricating properties of polyelectrolyte brushes in multivalent solution are hindered relative to those in monovalent solution.
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- Findingreasoning
The presence of multivalent ions (Y3+, Ca2+, Ba2+), even at minute concentrations, dramatically increases the friction forces between polyelectrolyte brush layers.
“The presence of multivalent ions (Y 3+ , Ca 2+ , Ba 2+ ), even at minute concentrations, dramatically increases the friction forces between brush layers due to electrostatic bridging and brush collapse.”
Quote in the paperSubstantial claim - Findingown data
The coefficient of friction between two PSS brush layers in 6 mM NaNO3 was smaller than 0.001.
“The coefficient of friction (COF), µ, between the two brush layers, defined as dFk/dL, was smaller than 0.001.”
Quote in the paperSubstantial claim - Findingown data
In 6 mM NaNO3, PSS brushes showed excellent lubrication properties.
“In 6 mM NaNO3, the PSS brushes showed excellent lubrication properties.”
Quote in the paperSubstantial claim - Findingown data
This work confirms that the charged polymer chains and the osmotic pressure of the counterions provide excellent lubrication properties in monovalent salt solution.
“This work confirms that the charged polymer chains and the osmotic pressure of the counterions provide excellent lubrication properties in monovalent salt solution.”
Quote in the paperSubstantial claim - Interpretationown data
The lubricating properties of polyelectrolyte brushes in multivalent solution are hindered relative to those in monovalent solution.
“Our results suggest the lubricating properties of polyelectrolyte brushes in multivalent solution are hindered relative to those in monovalent solution.”
Quote in the paperSubstantial claim
- Interpretationown data
The increase in friction forces between polyelectrolyte brush layers in multivalent solution is due to electrostatic bridging and brush collapse.
“The presence of multivalent ions (Y 3+ , Ca 2+ , Ba 2+ ), even at minute concentrations, dramatically increases the friction forces between brush layers due to electrostatic bridging and brush collapse.”
Quote in the paperSubstantial claim - Interpretationown data
Simulation results support the hypothesis that structural change of the polyelectrolyte brushes dominates the friction at much higher concentrations.
“Simulation results support the hypothesis that electrostatic bridging increases the friction between apposing polyelectrolyte brushes at low multivalent ion concentrations (Fig. 4B,C), and that structural change of the polyelectrolyte brushes dominates the friction at much higher concentrations (Fig. 4D).”
Quote in the paperSubstantial claim- Rests on an assumption: The coarse-grained MD simulations accurately capture the structural and bridging behavior of PSS brushes with multivalent ions.
- Interpretationown data
At high concentrations of multivalent salt, the brushes undergo a heterogeneous collapse resulting in increased surface roughness.
“(2) at high concentrations of multivalent salt, the brushes undergo a heterogeneous collapse resulting in increased surface roughness.”
Quote in the paperSubstantial claim - Interpretationown data
Simulation results support the hypothesis that electrostatic bridging increases the friction between apposing polyelectrolyte brushes at low multivalent ion concentrations.
“Simulation results support the hypothesis that electrostatic bridging increases the friction between apposing polyelectrolyte brushes at low multivalent ion concentrations (Fig. 4B,C), and that structural change of the polyelectrolyte brushes dominates the friction at much higher concentrations (Fig. 4D).”
Quote in the paperSubstantial claim- Rests on an assumption: The coarse-grained MD simulations accurately capture the structural and bridging behavior of PSS brushes with multivalent ions.
- May combine two claims. 5
- Classified as probably not a substantial claim. 4
May combine two claims.
Findingown dataIn the 0.5 mM Y3+ solution, the coefficient of friction was in the range 0.15-0.3, two orders of magnitude larger than in 6 mM NaNO3.
“µ was in the range 0.15-0.3,two orders of magnitude larger than in 6 mM NaNO3.”
Quote in the paperSubstantial claimMay combine two claims.
Findingown dataAFM measurements confirmed that in 0.1 and 0.5 mM Y3+, and 1 mM Ba2+ solution, the brush layer collapsed into pinned-micelle like structures accompanied by a stark decrease in brush height.
“AFM measurements confirmed that in 0.1 and 0.5 mM Y 3+ , and 1 mM Ba 2+ solution, the brush layer collapsed into pinned-micelle like structures (Figs.2C,D, S10-S12) accompanied by a stark decrease in brush height (Figs.2E, S2, S8).”
Quote in the paperSubstantial claimMay combine two claims.
Findingown dataThe addition of 0.01 mM Y3+ significantly affected the friction force, which was very small at loads up to 3 mN, and then rapidly increased.
“However, the addition of 0.01 mM Y 3+ significantly affected the friction force (Fig. 1D), which was very small at loads up to 3 mN, and then rapidly increased.”
Quote in the paperSubstantial claimMay combine two claims.
Interpretationown dataThe agreement between SFA and AFM measurements shows that multivalent counterions dramatically influence the structure and mechanical properties of the PSS brushes, dictating their boundary lubrication properties.
“The agreement between SFA and AFM measurements show that multivalent counterions dramatically influence the structure and mechanical properties of the PSS brushes, dictating their boundary lubrication properties (Fig. 2E and Fig. S13).”
Quote in the paperSubstantial claimClassified as probably not a substantial claim.
Interpretationown dataAt low concentrations of multivalent salt, multivalency induces three-body electrostatic bridging interactions between PSS chains.
“(1) At low concentrations of multivalent salt, multivalency induces three-body electrostatic bridging interactions between PSS chains”
Quote in the paperSubstantial claimMay combine two claims.
Interpretationown dataThe lubrication of polyelectrolyte brushes can break down in the presence of multivalent counterions, even at very low concentrations, resulting from electrostatic bridging between chains from apposing surfaces and changes in surface topology.
“However, the lubrication can break down in the presence of multivalent counterions, even at very low concentrations, resulting from electrostatic bridging between chains from apposing surfaces and changes in surface topology.”
Quote in the paperSubstantial claimProbably not a substantial claim: may not pass S1 (asserted).
InterpretationcitationThe increase in friction force at 0.01 mM Y3+ above 3 mN load is due to enhanced chain interpenetration of the apposing brushes at higher compression, leading to more bridging events between negatively charged sulfonate groups mediated by multivalent ions.
“We hypothesize that this increase was due to enhanced chain interpenetration of the apposing brushes at higher compression (31), leading to more bridging events between the negatively charged sulfonate groups, mediated by the multivalent ions.”
Quote in the paperNot a substantial claim0 of 1 sources checked- cites [31] 31. M. Ruths, D. Johannsmann, J. Ruhe, W. Knoll, Macromolecules 33, 3860-3870 (2000).
Couldn’t be matched to a paper in Crossref, so it can’t be checked.
Probably not a substantial claim: may not pass S3 (load-bearing).
Study design and conductnone givenError bars represent +/-SD, averaged over six to ten repeat measurements.
“Error bars represent +/-SD, averaged over six to ten repeat measurements.”
Quote in the paperNot a substantial claimProbably not a substantial claim: may not pass S3 (load-bearing).
Study design and conductnone givenNo damage was detected during the friction measurements.
“No damage was detected during the friction measurements.”
Quote in the paperNot a substantial claim
The paper relies on this without support.
PSS brushes are representative of polyelectrolyte brushes in biological and industrial contexts.
“Our discoveries have implications for developing better water-based boundary lubrication for manmade systems in aqueous or physiological media, such as in biomedical devices.”
The paper relies on this without support.
The coarse-grained MD simulations accurately capture the structural and bridging behavior of PSS brushes with multivalent ions.
“Coarse-grained molecular dynamics (MD) simulations of polyelectrolyte brushes in the SFA geometry were employed to investigate these hypotheses.”
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Effects of Ion Valency on Polyelectrolyte Brushes: A Unified Theory
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Electrostatic Correlation Induced Ion Condensation and Charge Inversion in Multivalent Electrolytes
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Constrained thermoresponsive polymers – new insights into fundamentals and applications
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Cartilage Lubrication from the Perspective of Wettability
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Control of Polymer Brush Morphology, Rheology, and Protein Repulsion by Hydrogen Bond Complexation
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Atomistic Insights into the Ionic Response and Mechanism of Antifouling Zwitterionic Polymer Brushes
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Nature of Overcharging and Charge Inversion in Electrical Double Layers
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Theoretical Modeling of Chemical Equilibrium in Weak Polyelectrolyte Layers on Curved Nanosystems
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Complex Coacervation in Asymmetric Solutions of Polycation and Polyanion
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Responsive Polyelectrolyte Brushes in Applications: Functions, Stimuli, and Design Considerations
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The Whole Is Greater than the Sum of Its Parts – Challenges and Perspectives in Polyelectrolytes
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- Authors
- Yu, J., Jackson, N. E., Xu, X., Morgenstern, Y., Kaufman, Y., Ruths, M., de Pablo, J. J., & Tirrell, M.
- Affiliations
- Argonne National Laboratory (US)
- University of Massachusetts Lowell (US)
- Ben-Gurion University of the Negev (IL)
- Institute for Molecular Engineering, University of Chicago, Chicago, IL 60637, USA.
- Corresponding author
- Yu, J.
- Jackson, N. E.
- Tirrell, M.
- Venue
- Science
- Published
- 2018-06-29
- Volume
- 360
- Issue
- 6396
- Pages
- 1434-1438
- ISSN
- 0036-8075 (ISSN-L)
- 1095-9203
- OpenAlex
- W2810687263
- Cited by
- 207
- References
- 39
- Citations by year
- 2026: 16 · 2025: 32 · 2024: 30 · 2023: 24 · 2022: 27 · 2021: 31 · 2020: 23 · 2019: 19 · 2018: 5
- FWCI
- 6.61
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Locations
- Science (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- DR-NTU (Nanyang Technological University) (submittedVersion)
- Funders
- U.S. Department of Energy Basic Energy Sciences
- Topics
- Physical Sciences › Materials Science › Surfaces, Coatings and Films › Polymer Surface Interaction Studies
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Electrostatics and Colloid Interactions
- Physical Sciences › Engineering › Mechanical Engineering › Lubricants and Their Additives
- Keywords
- polyelectrolyte brushes, multivalent counterions, brush collapse, friction, lubrication, biomedical devices
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