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Polymers 2017, 9(8), 324; https://doi.org/10.3390/polym9080324

Probing the Nanoscopic Thermodynamic Fingerprint of Paramagnetic Ligands Interacting with Amphiphilic Macromolecules

Institute of Chemistry, Martin-Luther-Universität Halle-Wittenberg, Von-Danckelmann-Platz 4, 06120 Halle, Germany
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Received: 5 July 2017 / Revised: 24 July 2017 / Accepted: 24 July 2017 / Published: 31 July 2017
(This article belongs to the Special Issue From Amphiphilic to Polyphilic Polymers)
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Abstract

Self-assembly of macromolecules with ligands is an intricate dynamic process that depends on a wide variety of parameters and forms the basis of many essential biological processes. We elucidate the underlying energetic processes of self-assembly in a model system consisting of amphiphilic core-shell polymers interacting with paramagnetic, amphiphilic ligand molecules from temperature-dependent continuous wave electron paramagnetic resonance (CW EPR) spectroscopy subsequent to spectral simulation. The involved processes as observed from the ligands’ point of view are either based on temperature-dependent association constants (KA,j,k) or dynamic rotational regime interconversion (IC) constants (KIC,j,k). The interconversion process describes a transition from Brownian (b1) towards free (b2) diffusion of ligand. Both processes exhibit non-linear van’t Hoff (lnK vs. T−1) plots in the temperature range of liquid water and we retrieve decisive dynamic information of the system from the energetic fingerprints of ligands on the nanoscale, especially from the temperature-dependent interconversion heat capacity (∆C°P,IC). View Full-Text
Keywords: amphiphilic polymers; core-shell polymers; ligand binding; ESR/EPR spectroscopy; binding thermodynamics amphiphilic polymers; core-shell polymers; ligand binding; ESR/EPR spectroscopy; binding thermodynamics
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Reichenwallner, J.; Schwieger, C.; Hinderberger, D. Probing the Nanoscopic Thermodynamic Fingerprint of Paramagnetic Ligands Interacting with Amphiphilic Macromolecules. Polymers 2017, 9, 324.

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