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A molecularly informed field-theoretic study of the complexation of polycation PDADMA with mixed micelles of sodium dodecyl sulfate and ethoxylated surfactants

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Abstract

The self-assembly and phase separation of mixtures of polyelectrolytes and surfactants are important to a range of applications, from formulating personal care products to drug encapsulation. In contrast to systems of oppositely charged polyelectrolytes, in polyelectrolyte-surfactant systems the surfactants micellize into structures that are highly responsive to solution conditions. In this work, we examine how the morphology of micelles and degree of polyelectrolyte adsorption dynamically change upon varying the mixing ratio of charged and neutral surfactants. Specifically, we consider a solution of the cationic polyelectrolyte polydiallyldimethylammonium, anionic surfactant sodium dodecyl sulfate, neutral ethoxylated surfactants (C\(_m\)EO\(_n\)), sodium chloride salt, and water. To capture the chemical specificity of these species, we leverage recent developments in constructing molecularly informed field theories via coarse-graining from all-atom simulations. Our results show how changing the surfactant mixing ratios and the identity of the nonionic surfactant modulates micelle size and surface charge, and as a result dictates the degree of polyelectrolyte adsorption. These results are in semi-quantitative agreement with experimental observations on the same system.

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Availability of data and materials

The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.

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  • 24 September 2023

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Acknowledgements

This work was supported by BASF Corporation through the California Research Alliance. We thank Keith Gutowski for generously sharing papers and engaging in insightful discussions with us. G.H.F. and K.T.D. also derived partial support from the National Science Foundation CMMT Program under grant number DMR-2104255. M.S.S. acknowledges funding support from the National Science Foundation through Award No. CHEM-1800344. K.S. also received support from the BioPACIFIC Materials Innovation Platform (NSF DMR-1933487). Use was made of computational facilities purchased with funds from the National Science Foundation (OAC-1925717) and administered by the Center for Scientific Computing (CSC). The CSC is supported by the California NanoSystems Institute and the Materials Research Science and Engineering Center (MRSEC; NSF DMR-2308708) at UC Santa Barbara.

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  1. My Nguyen and Kevin Shen have contributed equally to this work.

Authors and Affiliations

  1. Department of Chemical Engineering, University of California, Santa Barbara, CA, 93106, USA

    My Nguyen, Kevin Shen, M. Scott Shell & Glenn H. Fredrickson

  2. BASF Corporation, Iselin, NJ, 08830, USA

    Nicholas Sherck

  3. BASF SE, 67056, Ludwigshafen am Rhein, Germany

    Stephan Köhler

  4. California Research Alliance (CARA) by BASF, Berkeley, CA, 94720, USA

    Rohini Gupta

  5. Materials Research Laboratory, University of California, Santa Barbara, CA, 93106, USA

    Kevin Shen, Kris T. Delaney & Glenn H. Fredrickson

  6. Department of Materials, University of California, Santa Barbara, CA, 93106, USA

    Glenn H. Fredrickson

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Contributions

MN and KS contributed to the conception, data acquisition and analysis, and writing of the manuscript. NS, SK, RG, KTD, MSS, and GHF contributed to the conception, review and editing of the manuscript, and funding acquisition.

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Correspondence to M. Scott Shell or Glenn H. Fredrickson.

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This article is dedicated to Fyl Pincus whose scientific achievements and mentoring in condensed and soft matter, polymers, polyelectrolytes, colloids, biological physics, and Coulombic effects have had a great impact on the research community.

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Nguyen, M., Shen, K., Sherck, N. et al. A molecularly informed field-theoretic study of the complexation of polycation PDADMA with mixed micelles of sodium dodecyl sulfate and ethoxylated surfactants. Eur. Phys. J. E 46, 75 (2023). https://doi.org/10.1140/epje/s10189-023-00332-4

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