Multivalent counterions diminish the lubricity of polyelectrolyte brushes

Yu, J.; Jackson, N. E.; Xu, X.; Morgenstern, Y.; Kaufman, Y.; Ruths, M.; de Pablo, J. J.; Tirrell, M.

doi:10.1126/science.aar5877

Title: Multivalent counterions diminish the lubricity of polyelectrolyte brushes

Journal Article · Fri Jun 29 00:00:00 EDT 2018 · Science

DOI:https://doi.org/10.1126/science.aar5877· OSTI ID:1463685

^[1];

^[2]; Xu, X. ^[3]; Morgenstern, Y. ^[4]; Kaufman, Y. ^[4];

^[3]; de Pablo, J. J. ^[2];

^[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)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1463685

Journal Information:: Science, Vol. 360, Issue 6396; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 102 works

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References (38)

Structure of Polyelectrolyte Brushes in the Presence of Multivalent Counterions Yu, Jing; Mao, Jun; Yuan, Guangcui Macromolecules, Vol. 49, Issue 15 https://doi.org/10.1021/acs.macromol.6b01064	journal	July 2016
DNA condensation in one dimension Pardatscher, Günther; Bracha, Dan; Daube, Shirley S. Nature Nanotechnology, Vol. 11, Issue 12 https://doi.org/10.1038/nnano.2016.142	journal	August 2016
Sweet, Hairy, Soft, and Slippery Lee, S.; Spencer, N. D. Science, Vol. 319, Issue 5863 https://doi.org/10.1126/science.1153273	journal	February 2008
Lubrication of Articular Cartilage Jahn, Sabrina; Seror, Jasmine; Klein, Jacob Annual Review of Biomedical Engineering, Vol. 18, Issue 1 https://doi.org/10.1146/annurev-bioeng-081514-123305	journal	July 2016
Repulsive Forces and Relaxation on Compression of Entangled, Polydisperse Polystyrene Brushes Ruths, Marina; Johannsmann, Diethelm; Rühe, Jürgen Macromolecules, Vol. 33, Issue 10 https://doi.org/10.1021/ma9920994	journal	May 2000
Surface and Interface Analyses of Polymer Brushes by Synchrotron Radiation Hoshino, Taiki; Tanaka, Yoshihito; Jinnai, Hiroshi Journal of the Physical Society of Japan, Vol. 82, Issue 2 https://doi.org/10.7566/JPSJ.82.021014	journal	February 2013
Controlled Synthesis of Polymer Brushes by “Living” Free Radical Polymerization Techniques Husseman, Marc; Malmström, Eva E.; McNamara, Molly Macromolecules, Vol. 32, Issue 5 https://doi.org/10.1021/ma981290v	journal	March 1999
Polyelectrolyte brushes: a novel stable lubrication system in aqueous conditions Kobayashi, Motoyasu; Terada, Masami; Takahara, Atsushi Faraday Discussions, Vol. 156 https://doi.org/10.1039/c2fd00123c	journal	January 2012
Electrochemical DNA sensors Drummond, T. Gregory; Hill, Michael G.; Barton, Jacqueline K. Nature Biotechnology, Vol. 21, Issue 10 https://doi.org/10.1038/nbt873	journal	October 2003
Counterion-induced condensation of deoxyribonucleic acid. A light-scattering study Wilson, Robert Wilfred; Bloomfield, Victor A. Biochemistry, Vol. 18, Issue 11 https://doi.org/10.1021/bi00578a009	journal	May 1979
Comparing Solvophobic and Multivalent Induced Collapse in Polyelectrolyte Brushes Jackson, Nicholas E.; Brettmann, Blair K.; Vishwanath, Venkatram ACS Macro Letters, Vol. 6, Issue 2 https://doi.org/10.1021/acsmacrolett.6b00837	journal	January 2017
Reversible Adhesion with Polyelectrolyte Brushes Tailored via the Uptake and Release of Trivalent Lanthanum Ions Farina, Robert; Laugel, Nicolas; Yu, Jing The Journal of Physical Chemistry C, Vol. 119, Issue 26 https://doi.org/10.1021/acs.jpcc.5b02121	journal	April 2015
Nanotribological properties of nanostructured poly(cysteine methacrylate) brushes Al-Jaf, Omed; Alswieleh, Abdullah; Armes, Steven P. Soft Matter, Vol. 13, Issue 10 https://doi.org/10.1039/C7SM00013H	journal	January 2017
Surface-Grafted, Covalently Cross-Linked Hydrogel Brushes with Tunable Interfacial and Bulk Properties Li, Ang; Benetti, Edmondo M.; Tranchida, Davide Macromolecules, Vol. 44, Issue 13 https://doi.org/10.1021/ma2006443	journal	July 2011
Dendritic and Nanowire Assemblies of Condensed DNA Polymer Brushes Bracha, Dan; Bar-Ziv, Roy H. Journal of the American Chemical Society, Vol. 136, Issue 13 https://doi.org/10.1021/ja410960w	journal	March 2014
Macrotribological Studies of Poly(L-lysine)-graft-Poly(ethylene glycol) in Aqueous Glycerol Mixtures Nalam, Prathima C.; Clasohm, Jarred N.; Mashaghi, Alireza Tribology Letters, Vol. 37, Issue 3 https://doi.org/10.1007/s11249-009-9549-9	journal	December 2009
Room-Temperature, Aqueous-Phase Fabrication of Poly(methacrylic acid) Brushes by UV-LED-Induced, Controlled Radical Polymerization with High Selectivity for Surface-Bound Species Heeb, Raphael; Bielecki, Robert M.; Lee, Seunghwan Macromolecules, Vol. 42, Issue 22 https://doi.org/10.1021/ma901607w	journal	November 2009
Supramolecular synergy in the boundary lubrication of synovial joints Seror, Jasmine; Zhu, Linyi; Goldberg, Ronit Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7497	journal	March 2015
Lubrication by charged polymers Raviv, Uri; Giasson, Suzanne; Kampf, Nir Nature, Vol. 425, Issue 6954 https://doi.org/10.1038/nature01970	journal	September 2003
Multivalent ions induce lateral structural inhomogeneities in polyelectrolyte brushes Yu, Jing; Jackson, Nicholas E.; Xu, Xin Science Advances, Vol. 3, Issue 12 https://doi.org/10.1126/sciadv.aao1497	journal	December 2017
Adsorption, Lubrication, and Wear of Lubricin on Model Surfaces: Polymer Brush-Like Behavior of a Glycoprotein Zappone, Bruno; Ruths, Marina; Greene, George W. Biophysical Journal, Vol. 92, Issue 5 https://doi.org/10.1529/biophysj.106.088799	journal	March 2007
Heterogeneous Morphology and Dynamics of Polyelectrolyte Brush Condensates in Trivalent Counterion Solution Liu, Lei; Pincus, Philip A.; Hyeon, Changbong Macromolecules, Vol. 50, Issue 4 https://doi.org/10.1021/acs.macromol.6b02685	journal	February 2017
Biomimetic engineering of non-adhesive glycocalyx-like surfaces using oligosaccharide surfactant polymers Holland, Nolan B.; Qiu, Yongxing; Ruegsegger, Mark Nature, Vol. 392, Issue 6678 https://doi.org/10.1038/33894	journal	April 1998
Lateral Structure Formation in Polyelectrolyte Brushes Induced by Multivalent Ions Brettmann, Blair; Pincus, Philip; Tirrell, Matthew Macromolecules, Vol. 50, Issue 3 https://doi.org/10.1021/acs.macromol.6b02563	journal	January 2017
Lubrication by Polyelectrolyte Brushes Zhulina, Ekaterina B.; Rubinstein, Michael Macromolecules, Vol. 47, Issue 16 https://doi.org/10.1021/ma500772a	journal	August 2014
Adhesion and Friction Mechanisms of Polymer-on-Polymer Surfaces Maeda, N. Science, Vol. 297, Issue 5580 https://doi.org/10.1126/science.1072378	journal	July 2002
Sacrificial bonds and hidden length dissipate energy as mineralized fibrils separate during bone fracture Fantner, Georg E.; Hassenkam, Tue; Kindt, Johannes H. Nature Materials, Vol. 4, Issue 8 https://doi.org/10.1038/nmat1428	journal	July 2005
Collapse of Spherical Polyelectrolyte Brushes in the Presence of Multivalent Counterions Mei, Yu; Lauterbach, Karlheinz; Hoffmann, Martin Physical Review Letters, Vol. 97, Issue 15 https://doi.org/10.1103/PhysRevLett.97.158301	journal	October 2006
The effect of multivalent counterions to the structure of highly dense polystyrene sulfonate brushes Yu, Jing; Mao, Jun; Yuan, Guangcui Polymer, Vol. 98 https://doi.org/10.1016/j.polymer.2016.02.053	journal	August 2016
Emerging applications of stimuli-responsive polymer materials Stuart, Martien A. Cohen; Huck, Wilhelm T. S.; Genzer, Jan Nature Materials, Vol. 9, Issue 2, p. 101-113 https://doi.org/10.1038/nmat2614	journal	January 2010
Tribology of surface-grafted polymer brushes Mocny, Piotr; Klok, Harm-Anton Molecular Systems Design & Engineering, Vol. 1, Issue 2 https://doi.org/10.1039/C5ME00010F	journal	January 2016
Bioinspired Bottle-Brush Polymer Exhibits Low Friction and Amontons-like Behavior Banquy, Xavier; Burdyńska, Joanna; Lee, Dong Woog Journal of the American Chemical Society, Vol. 136, Issue 17 https://doi.org/10.1021/ja501770y	journal	April 2014
Colloid stabilization with grafted polyelectrolytes Pincus, Philip Macromolecules, Vol. 24, Issue 10 https://doi.org/10.1021/ma00010a043	journal	May 1991
Programmable on-chip DNA compartments as artificial cells Karzbrun, E.; Tayar, A. M.; Noireaux, V. Science, Vol. 345, Issue 6198 https://doi.org/10.1126/science.1255550	journal	August 2014
Shear, Friction, and Lubrication Forces Between Polymer-Bearing Surfaces Klein, J. Annual Review of Materials Science, Vol. 26, Issue 1 https://doi.org/10.1146/annurev.ms.26.080196.003053	journal	August 1996
Lubrication at Physiological Pressures by Polyzwitterionic Brushes Chen, M.; Briscoe, W. H.; Armes, S. P. Science, Vol. 323, Issue 5922 https://doi.org/10.1126/science.1169399	journal	March 2009
Structure formation in polyelectrolytes induced by multivalent ions Jusufi, Arben; Borisov, Oleg; Ballauff, Matthias Polymer, Vol. 54, Issue 8 https://doi.org/10.1016/j.polymer.2012.12.030	journal	April 2013
Synthesis and Swelling Behavior of pH-Responsive Polybase Brushes Sanjuan, S.; Perrin, P.; Pantoustier, N. Langmuir, Vol. 23, Issue 10 https://doi.org/10.1021/la063450z	journal	May 2007

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Investigating the effect of mono‐ and multivalent counterions on the conformation of poly(styrenesulfonic acid) by nanopores Zhao, Yating; Liu, Lei; Tu, Yingfeng ELECTROPHORESIS, Vol. 40, Issue 16-17 https://doi.org/10.1002/elps.201800539	journal	March 2019
The effects of grafting density and charge fraction on the properties of ring polyelectrolyte brushes: a molecular dynamics simulation study Hao, Qing-Hai; Liu, Li-Xiang; Xia, Gang Colloid and Polymer Science, Vol. 298, Issue 1 https://doi.org/10.1007/s00396-019-04579-2	journal	November 2019
Influence of divalent counterions on the solution rheology and supramolecular aggregation of carboxymethyl cellulose Lopez, Carlos G.; Richtering, Walter Cellulose, Vol. 26, Issue 3 https://doi.org/10.1007/s10570-018-2158-8	journal	December 2018
Surface morphologies of spherical polyelectrolyte brushes induced by trivalent salt ions Hao, Qing-Hai; Xia, Gang; Tan, Hong-Ge Physical Chemistry Chemical Physics, Vol. 20, Issue 41 https://doi.org/10.1039/c8cp04235g	journal	January 2018
Tuning phase transitions of aqueous protein solutions by multivalent cations Matsarskaia, Olga; Roosen-Runge, Felix; Lotze, Gudrun Physical Chemistry Chemical Physics, Vol. 20, Issue 42 https://doi.org/10.1039/c8cp05884a	journal	January 2018
Multivalent counterions accumulate in star-like polyelectrolytes and collapse the polymer in spite of increasing its ionization Staňo, Roman; Nová, Lucie; Uhlík, Filip Soft Matter, Vol. 16, Issue 4 https://doi.org/10.1039/c9sm02318f	journal	January 2020
Tardigrade inspired polyelectrolyte complexation and functional materials Zhang, Fang; Song, Changyuan; Zhu, Xiangwei Journal of Materials Chemistry A, Vol. 7, Issue 48 https://doi.org/10.1039/c9ta10931e	journal	January 2019
An in situ shearing x-ray measurement system for exploring structures and dynamics at the solid–liquid interface Qiao, Yijun; Zhou, Hua; Jiang, Zhang Review of Scientific Instruments, Vol. 91, Issue 1 https://doi.org/10.1063/1.5129819	journal	January 2020
Depletion layer dynamics of polyelectrolyte solutions under Poiseuille flow Park, Seong Jun; Shakya, Anisha; King, John T. Proceedings of the National Academy of Sciences, Vol. 116, Issue 33 https://doi.org/10.1073/pnas.1900623116	journal	July 2019
Polydopamine-Assisted Immobilization of Chitosan Brushes on a Textured CoCrMo Alloy to Improve its Tribology and Biocompatibility Qin, Liguo; Sun, Hongjiang; Hafezi, Mahshid Materials, Vol. 12, Issue 18 https://doi.org/10.3390/ma12183014	journal	September 2019
Wetting Behavior and Tribological Properties of Polymer Brushes on Laser-Textured Surface Shen, Ming-xue; Zhang, Zhao-xiang; Yang, Jin-tao Polymers, Vol. 11, Issue 6 https://doi.org/10.3390/polym11060981	journal	June 2019
Combined Experimental and Theoretical Study of Weak Polyelectrolyte Brushes in Salt Mixtures Willott, Joshua D.; Humphreys, Ben A.; Webber, Grant B. Langmuir, Vol. 35, Issue 7 https://doi.org/10.1021/acs.langmuir.8b03838	journal	January 2019

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