Determination of Hydrophobic Polymer Clustering in Concentrated Aqueous Solutions through Single-Particle Tracking Diffusion Studies

Harrison Landfield; Muzhou Wang

doi:10.1021/acs.macromol.2c00840

Determination of Hydrophobic Polymer Clustering in Concentrated Aqueous Solutions through Single-Particle Tracking Diffusion Studies

Harrison Landfield, Muzhou Wang^*

^*Corresponding author for this work

Chemical and Biological Engineering

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Noncovalent interactions allow associating polymers to self-assemble into structures that assist in applications such as contaminant removal and drug delivery. Using single-particle tracking (SPT) diffusion studies, we show that poly(ethylene glycol monomethacrylate) (pPEGMA) is a hydrophobically associating polymer, where polymer chains may diffuse individually or in clusters. Aided by the single-molecule resolution of SPT, we observe that the mean-squared displacements of pPEGMA chains in solution show a clear two-population division, which corresponds to unimers and clusters in our hypothesis. This bifurcation is also seen in the distributions of polymer mean-squared displacements and the van Hove distributions. Clustering behavior can be tuned by altering the concentration and molecular weight of the polymer, as well as the polarity of the solvent. Combined with dynamic light scattering (DLS) and diffusion ordered spectroscopy (DOSY), polymer diffusive regimes up to the semidilute entangled regime are experimentally observed.

Original language	English (US)
Pages (from-to)	7425-7437
Number of pages	13
Journal	Macromolecules
Volume	55
Issue number	17
DOIs	https://doi.org/10.1021/acs.macromol.2c00840
State	Published - Sep 13 2022

Funding

The authors are grateful to Drs. Angelika Neitzel and Jack Douglas; Profs. Julia Kalow, Jeffrey Richards, and Matthew Tirrell; and Kaden Stevens for access to their equipment and useful discussions. This work was performed under the financial assistance award 70NANB14H012 from U.S. Department of Commerce, National Institute of Standards and Technology, as part of the Center for Hierarchical Materials Design (CHiMaD). This work made use of the IMSERC NMR and Keck-II facilities of the NUANCE Center at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), Int. Institute of Nanotechnology, Northwestern’s MRSEC program (NSF DMR-1720139), and Northwestern University.

ASJC Scopus subject areas

Organic Chemistry
Polymers and Plastics
Inorganic Chemistry
Materials Chemistry

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10.1021/acs.macromol.2c00840

Cite this

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title = "Determination of Hydrophobic Polymer Clustering in Concentrated Aqueous Solutions through Single-Particle Tracking Diffusion Studies",

abstract = "Noncovalent interactions allow associating polymers to self-assemble into structures that assist in applications such as contaminant removal and drug delivery. Using single-particle tracking (SPT) diffusion studies, we show that poly(ethylene glycol monomethacrylate) (pPEGMA) is a hydrophobically associating polymer, where polymer chains may diffuse individually or in clusters. Aided by the single-molecule resolution of SPT, we observe that the mean-squared displacements of pPEGMA chains in solution show a clear two-population division, which corresponds to unimers and clusters in our hypothesis. This bifurcation is also seen in the distributions of polymer mean-squared displacements and the van Hove distributions. Clustering behavior can be tuned by altering the concentration and molecular weight of the polymer, as well as the polarity of the solvent. Combined with dynamic light scattering (DLS) and diffusion ordered spectroscopy (DOSY), polymer diffusive regimes up to the semidilute entangled regime are experimentally observed.",

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N2 - Noncovalent interactions allow associating polymers to self-assemble into structures that assist in applications such as contaminant removal and drug delivery. Using single-particle tracking (SPT) diffusion studies, we show that poly(ethylene glycol monomethacrylate) (pPEGMA) is a hydrophobically associating polymer, where polymer chains may diffuse individually or in clusters. Aided by the single-molecule resolution of SPT, we observe that the mean-squared displacements of pPEGMA chains in solution show a clear two-population division, which corresponds to unimers and clusters in our hypothesis. This bifurcation is also seen in the distributions of polymer mean-squared displacements and the van Hove distributions. Clustering behavior can be tuned by altering the concentration and molecular weight of the polymer, as well as the polarity of the solvent. Combined with dynamic light scattering (DLS) and diffusion ordered spectroscopy (DOSY), polymer diffusive regimes up to the semidilute entangled regime are experimentally observed.

AB - Noncovalent interactions allow associating polymers to self-assemble into structures that assist in applications such as contaminant removal and drug delivery. Using single-particle tracking (SPT) diffusion studies, we show that poly(ethylene glycol monomethacrylate) (pPEGMA) is a hydrophobically associating polymer, where polymer chains may diffuse individually or in clusters. Aided by the single-molecule resolution of SPT, we observe that the mean-squared displacements of pPEGMA chains in solution show a clear two-population division, which corresponds to unimers and clusters in our hypothesis. This bifurcation is also seen in the distributions of polymer mean-squared displacements and the van Hove distributions. Clustering behavior can be tuned by altering the concentration and molecular weight of the polymer, as well as the polarity of the solvent. Combined with dynamic light scattering (DLS) and diffusion ordered spectroscopy (DOSY), polymer diffusive regimes up to the semidilute entangled regime are experimentally observed.

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Determination of Hydrophobic Polymer Clustering in Concentrated Aqueous Solutions through Single-Particle Tracking Diffusion Studies

Abstract

Funding

ASJC Scopus subject areas

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