Multivalent counterions diminish the lubricity of polyelectrolyte brushes

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Science  29 Jun 2018:
Vol. 360, Issue 6396, pp. 1434-1438
DOI: 10.1126/science.aar5877

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A brush with friction

Polyelectrolyte brushes consist of charged polymer chains attached to a common backbone or surface. They provide excellent lubrication between two surfaces for both engineered and physiological materials. The packing of the brushes is sensitive to pH, temperature, or added salts. Yu et al. show that the presence of multivalent ions can cause brush collapse, similarly to monovalent ions (see the Perspective by Ballauff). Critically—and not observed with the addition of monovalent ions—very low concentrations of multivalent ions cause bridging between the brushes and increase friction between the surfaces to the extent that their value for biomedical devices is limited.

Science, this issue p. 1434; see also p. 1399


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. 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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