Journal
POLYMERS
Volume 9, Issue 8, Pages -Publisher
MDPI AG
DOI: 10.3390/polym9080324
Keywords
amphiphilic polymers; core-shell polymers; ligand binding; ESR/EPR spectroscopy; binding thermodynamics
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [HI 1094/5-1]
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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 (K-A,K-j,K-k) or dynamic rotational regime interconversion (IC) constants (K-IC,K- (j,) (k)). The interconversion process describes a transition from Brownian (b(1)) towards free (b(2)) 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 (Delta C degrees (P,IC)).
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