Multivalent counterions diminish the lubricity of polyelectrolyte brushes
Abstract
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, markedly increases the friction forces between brush layers owing to electrostatic bridging and brush collapse. Furthermore, our results suggest that the lubricating properties of polyelectrolyte brushes in multivalent solution are hindered relative to those in monovalent solution.
- Authors:
-
[1];
[2];
[3];
[2]
- Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States); Nanyang Technological Univ. (Singapore)
- Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Univ. of Massachusetts, Lowell, MA (United States)
- Ben-Gurion Univ. of the Negev, Midreshet Ben-Gurion (Israel)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1463685
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science
- Additional Journal Information:
- Journal Volume: 360; Journal Issue: 6396; Journal ID: ISSN 0036-8075
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 47 OTHER INSTRUMENTATION
Citation Formats
Yu, J., Jackson, N. E., Xu, X., Morgenstern, Y., Kaufman, Y., Ruths, M., de Pablo, J. J., and Tirrell, M. Multivalent counterions diminish the lubricity of polyelectrolyte brushes. United States: N. p., 2018.
Web. doi:10.1126/science.aar5877.
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. United States. https://doi.org/10.1126/science.aar5877
Yu, J., Jackson, N. E., Xu, X., Morgenstern, Y., Kaufman, Y., Ruths, M., de Pablo, J. J., and Tirrell, M. Fri .
"Multivalent counterions diminish the lubricity of polyelectrolyte brushes". United States. https://doi.org/10.1126/science.aar5877. https://www.osti.gov/servlets/purl/1463685.
@article{osti_1463685,
title = {Multivalent counterions diminish the lubricity of polyelectrolyte brushes},
author = {Yu, J. and Jackson, N. E. and Xu, X. and Morgenstern, Y. and Kaufman, Y. and Ruths, M. and de Pablo, J. J. and Tirrell, M.},
abstractNote = {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, markedly increases the friction forces between brush layers owing to electrostatic bridging and brush collapse. Furthermore, our results suggest that the lubricating properties of polyelectrolyte brushes in multivalent solution are hindered relative to those in monovalent solution.},
doi = {10.1126/science.aar5877},
journal = {Science},
number = 6396,
volume = 360,
place = {United States},
year = {Fri Jun 29 00:00:00 EDT 2018},
month = {Fri Jun 29 00:00:00 EDT 2018}
}
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Works referenced in this record:
Structure of Polyelectrolyte Brushes in the Presence of Multivalent Counterions
journal, July 2016
- Yu, Jing; Mao, Jun; Yuan, Guangcui
- Macromolecules, Vol. 49, Issue 15
DNA condensation in one dimension
journal, August 2016
- Pardatscher, Günther; Bracha, Dan; Daube, Shirley S.
- Nature Nanotechnology, Vol. 11, Issue 12
Sweet, Hairy, Soft, and Slippery
journal, February 2008
- Lee, S.; Spencer, N. D.
- Science, Vol. 319, Issue 5863
Lubrication of Articular Cartilage
journal, July 2016
- Jahn, Sabrina; Seror, Jasmine; Klein, Jacob
- Annual Review of Biomedical Engineering, Vol. 18, Issue 1
Repulsive Forces and Relaxation on Compression of Entangled, Polydisperse Polystyrene Brushes
journal, May 2000
- Ruths, Marina; Johannsmann, Diethelm; Rühe, Jürgen
- Macromolecules, Vol. 33, Issue 10
Surface and Interface Analyses of Polymer Brushes by Synchrotron Radiation
journal, February 2013
- Hoshino, Taiki; Tanaka, Yoshihito; Jinnai, Hiroshi
- Journal of the Physical Society of Japan, Vol. 82, Issue 2
Controlled Synthesis of Polymer Brushes by “Living” Free Radical Polymerization Techniques
journal, March 1999
- Husseman, Marc; Malmström, Eva E.; McNamara, Molly
- Macromolecules, Vol. 32, Issue 5
Polyelectrolyte brushes: a novel stable lubrication system in aqueous conditions
journal, January 2012
- Kobayashi, Motoyasu; Terada, Masami; Takahara, Atsushi
- Faraday Discussions, Vol. 156
Electrochemical DNA sensors
journal, October 2003
- Drummond, T. Gregory; Hill, Michael G.; Barton, Jacqueline K.
- Nature Biotechnology, Vol. 21, Issue 10
Counterion-induced condensation of deoxyribonucleic acid. A light-scattering study
journal, May 1979
- Wilson, Robert Wilfred; Bloomfield, Victor A.
- Biochemistry, Vol. 18, Issue 11
Comparing Solvophobic and Multivalent Induced Collapse in Polyelectrolyte Brushes
journal, January 2017
- Jackson, Nicholas E.; Brettmann, Blair K.; Vishwanath, Venkatram
- ACS Macro Letters, Vol. 6, Issue 2
Reversible Adhesion with Polyelectrolyte Brushes Tailored via the Uptake and Release of Trivalent Lanthanum Ions
journal, April 2015
- Farina, Robert; Laugel, Nicolas; Yu, Jing
- The Journal of Physical Chemistry C, Vol. 119, Issue 26
Nanotribological properties of nanostructured poly(cysteine methacrylate) brushes
journal, January 2017
- Al-Jaf, Omed; Alswieleh, Abdullah; Armes, Steven P.
- Soft Matter, Vol. 13, Issue 10
Surface-Grafted, Covalently Cross-Linked Hydrogel Brushes with Tunable Interfacial and Bulk Properties
journal, July 2011
- Li, Ang; Benetti, Edmondo M.; Tranchida, Davide
- Macromolecules, Vol. 44, Issue 13
Dendritic and Nanowire Assemblies of Condensed DNA Polymer Brushes
journal, March 2014
- Bracha, Dan; Bar-Ziv, Roy H.
- Journal of the American Chemical Society, Vol. 136, Issue 13
Macrotribological Studies of Poly(L-lysine)-graft-Poly(ethylene glycol) in Aqueous Glycerol Mixtures
journal, December 2009
- Nalam, Prathima C.; Clasohm, Jarred N.; Mashaghi, Alireza
- Tribology Letters, Vol. 37, Issue 3
Room-Temperature, Aqueous-Phase Fabrication of Poly(methacrylic acid) Brushes by UV-LED-Induced, Controlled Radical Polymerization with High Selectivity for Surface-Bound Species
journal, November 2009
- Heeb, Raphael; Bielecki, Robert M.; Lee, Seunghwan
- Macromolecules, Vol. 42, Issue 22
Supramolecular synergy in the boundary lubrication of synovial joints
journal, March 2015
- Seror, Jasmine; Zhu, Linyi; Goldberg, Ronit
- Nature Communications, Vol. 6, Issue 1
Lubrication by charged polymers
journal, September 2003
- Raviv, Uri; Giasson, Suzanne; Kampf, Nir
- Nature, Vol. 425, Issue 6954
Multivalent ions induce lateral structural inhomogeneities in polyelectrolyte brushes
journal, December 2017
- Yu, Jing; Jackson, Nicholas E.; Xu, Xin
- Science Advances, Vol. 3, Issue 12
Adsorption, Lubrication, and Wear of Lubricin on Model Surfaces: Polymer Brush-Like Behavior of a Glycoprotein
journal, March 2007
- Zappone, Bruno; Ruths, Marina; Greene, George W.
- Biophysical Journal, Vol. 92, Issue 5
Heterogeneous Morphology and Dynamics of Polyelectrolyte Brush Condensates in Trivalent Counterion Solution
journal, February 2017
- Liu, Lei; Pincus, Philip A.; Hyeon, Changbong
- Macromolecules, Vol. 50, Issue 4
Biomimetic engineering of non-adhesive glycocalyx-like surfaces using oligosaccharide surfactant polymers
journal, April 1998
- Holland, Nolan B.; Qiu, Yongxing; Ruegsegger, Mark
- Nature, Vol. 392, Issue 6678
Lateral Structure Formation in Polyelectrolyte Brushes Induced by Multivalent Ions
journal, January 2017
- Brettmann, Blair; Pincus, Philip; Tirrell, Matthew
- Macromolecules, Vol. 50, Issue 3
Lubrication by Polyelectrolyte Brushes
journal, August 2014
- Zhulina, Ekaterina B.; Rubinstein, Michael
- Macromolecules, Vol. 47, Issue 16
Adhesion and Friction Mechanisms of Polymer-on-Polymer Surfaces
journal, July 2002
- Maeda, N.
- Science, Vol. 297, Issue 5580
Sacrificial bonds and hidden length dissipate energy as mineralized fibrils separate during bone fracture
journal, July 2005
- Fantner, Georg E.; Hassenkam, Tue; Kindt, Johannes H.
- Nature Materials, Vol. 4, Issue 8
Collapse of Spherical Polyelectrolyte Brushes in the Presence of Multivalent Counterions
journal, October 2006
- Mei, Yu; Lauterbach, Karlheinz; Hoffmann, Martin
- Physical Review Letters, Vol. 97, Issue 15
The effect of multivalent counterions to the structure of highly dense polystyrene sulfonate brushes
journal, August 2016
- Yu, Jing; Mao, Jun; Yuan, Guangcui
- Polymer, Vol. 98
Emerging applications of stimuli-responsive polymer materials
journal, January 2010
- Stuart, Martien A. Cohen; Huck, Wilhelm T. S.; Genzer, Jan
- Nature Materials, Vol. 9, Issue 2, p. 101-113
Tribology of surface-grafted polymer brushes
journal, January 2016
- Mocny, Piotr; Klok, Harm-Anton
- Molecular Systems Design & Engineering, Vol. 1, Issue 2
Bioinspired Bottle-Brush Polymer Exhibits Low Friction and Amontons-like Behavior
journal, April 2014
- Banquy, Xavier; Burdyńska, Joanna; Lee, Dong Woog
- Journal of the American Chemical Society, Vol. 136, Issue 17
Colloid stabilization with grafted polyelectrolytes
journal, May 1991
- Pincus, Philip
- Macromolecules, Vol. 24, Issue 10
Programmable on-chip DNA compartments as artificial cells
journal, August 2014
- Karzbrun, E.; Tayar, A. M.; Noireaux, V.
- Science, Vol. 345, Issue 6198
Shear, Friction, and Lubrication Forces Between Polymer-Bearing Surfaces
journal, August 1996
- Klein, J.
- Annual Review of Materials Science, Vol. 26, Issue 1
Lubrication at Physiological Pressures by Polyzwitterionic Brushes
journal, March 2009
- Chen, M.; Briscoe, W. H.; Armes, S. P.
- Science, Vol. 323, Issue 5922
Structure formation in polyelectrolytes induced by multivalent ions
journal, April 2013
- Jusufi, Arben; Borisov, Oleg; Ballauff, Matthias
- Polymer, Vol. 54, Issue 8
Synthesis and Swelling Behavior of pH-Responsive Polybase Brushes
journal, May 2007
- Sanjuan, S.; Perrin, P.; Pantoustier, N.
- Langmuir, Vol. 23, Issue 10
Works referencing / citing this record:
Recent Advances in Bioinspired Gel Surfaces with Superwettability and Special Adhesion
journal, July 2019
- Zhang, Pengchao; Zhao, Chuangqi; Zhao, Tianyi
- Advanced Science, Vol. 6, Issue 18
Investigating the effect of mono‐ and multivalent counterions on the conformation of poly(styrenesulfonic acid) by nanopores
journal, March 2019
- Zhao, Yating; Liu, Lei; Tu, Yingfeng
- ELECTROPHORESIS, Vol. 40, Issue 16-17
The effects of grafting density and charge fraction on the properties of ring polyelectrolyte brushes: a molecular dynamics simulation study
journal, November 2019
- Hao, Qing-Hai; Liu, Li-Xiang; Xia, Gang
- Colloid and Polymer Science, Vol. 298, Issue 1
Influence of divalent counterions on the solution rheology and supramolecular aggregation of carboxymethyl cellulose
journal, December 2018
- Lopez, Carlos G.; Richtering, Walter
- Cellulose, Vol. 26, Issue 3
Surface morphologies of spherical polyelectrolyte brushes induced by trivalent salt ions
journal, January 2018
- Hao, Qing-Hai; Xia, Gang; Tan, Hong-Ge
- Physical Chemistry Chemical Physics, Vol. 20, Issue 41
Tuning phase transitions of aqueous protein solutions by multivalent cations
journal, January 2018
- Matsarskaia, Olga; Roosen-Runge, Felix; Lotze, Gudrun
- Physical Chemistry Chemical Physics, Vol. 20, Issue 42
Multivalent counterions accumulate in star-like polyelectrolytes and collapse the polymer in spite of increasing its ionization
journal, January 2020
- Staňo, Roman; Nová, Lucie; Uhlík, Filip
- Soft Matter, Vol. 16, Issue 4
Tardigrade inspired polyelectrolyte complexation and functional materials
journal, January 2019
- Zhang, Fang; Song, Changyuan; Zhu, Xiangwei
- Journal of Materials Chemistry A, Vol. 7, Issue 48
An in situ shearing x-ray measurement system for exploring structures and dynamics at the solid–liquid interface
journal, January 2020
- Qiao, Yijun; Zhou, Hua; Jiang, Zhang
- Review of Scientific Instruments, Vol. 91, Issue 1
Depletion layer dynamics of polyelectrolyte solutions under Poiseuille flow
journal, July 2019
- Park, Seong Jun; Shakya, Anisha; King, John T.
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 33
Polydopamine-Assisted Immobilization of Chitosan Brushes on a Textured CoCrMo Alloy to Improve its Tribology and Biocompatibility
journal, September 2019
- Qin, Liguo; Sun, Hongjiang; Hafezi, Mahshid
- Materials, Vol. 12, Issue 18
Wetting Behavior and Tribological Properties of Polymer Brushes on Laser-Textured Surface
journal, June 2019
- Shen, Ming-xue; Zhang, Zhao-xiang; Yang, Jin-tao
- Polymers, Vol. 11, Issue 6
Combined Experimental and Theoretical Study of Weak Polyelectrolyte Brushes in Salt Mixtures
journal, January 2019
- Willott, Joshua D.; Humphreys, Ben A.; Webber, Grant B.
- Langmuir, Vol. 35, Issue 7
Polydopamine-Assisted Immobilization of Chitosan Brushes on a Textured CoCrMo Alloy to Improve its Tribology and Biocompatibility
journal, September 2019
- Qin, Liguo; Sun, Hongjiang; Hafezi, Mahshid
- Materials, Vol. 12, Issue 18
Wetting Behavior and Tribological Properties of Polymer Brushes on Laser-Textured Surface
journal, June 2019
- Shen, Ming-xue; Zhang, Zhao-xiang; Yang, Jin-tao
- Polymers, Vol. 11, Issue 6