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Published May 11, 2021 | Supplemental Material
Journal Article Open

Nonelectrostatic Adsorption of Polyelectrolytes and Mediated Interactions between Solid Surfaces


Polymer-mediated interaction between two solid surfaces is directly connected to the properties of the adsorbed polymer layers. Nonelectrostatic interactions with a surface can significantly impact the adsorption of polyelectrolytes to charged surfaces. We use a classical density functional theory to study the effect of various polyelectrolyte solution properties on the adsorption and interaction between two like-charged surfaces. Our results show that nonelectrostatic interactions not only enhance polyelectrolyte adsorption but can also result in qualitatively different salt effects with respect to the adsorbed amount. In particular, we observe decreasing, increasing, and a previously unreported nonmonotonic behavior in the adsorbed amount of polymer with added salt under the conditions studied, although the nonmonotonic regime only occurs for a narrow range in the parameter space. With sufficient nonelectrostatic adsorption, the adsorbed polymer layers produce a long-range repulsive barrier that is strong enough to overcome dispersive interactions that cause surfaces to attract. Concurrently, a short-range bridging attraction is observed when the two polyelectrolyte layers span both the surfaces. Both the repulsive barrier and bridging attraction depend on the charge density of the polymer backbone and the bulk salt concentration but not on the chain length in the semidilute regime studied.

Additional Information

© 2021 American Chemical Society. Received: January 15, 2021; Revised: April 14, 2021; Published: April 29, 2021. The Dow Chemical Company is acknowledged for partly funding the work and permission to publish the results. C.B. is supported by the U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, Department of Energy Computational Science Graduate Fellowship under Award Number DE-SC0020347. We thank Dr. Chang Yun Son, Dr. Anthony Van Dyk, Dr. Thomas Kalantar, and Dr. Christopher Tucker for helpful discussions. Author Contributions. C.B. and J.J. contributed equally. The authors declare no competing financial interest.

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August 20, 2023
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