Theoretical investigation of charge effects on the critical solution temperature of thermosensitive, random copolymers
Final Report Abstract
The key achievements of this project can be summarized as follows. Based on a combination of experiments and atomistic and coarse-grained computer simulations, we have developed relatively simple mean field equations that can be readily applied to predict the influence of charge copolymerization and ion-specific screening on the coil-to-globule transition (or critical solution temperature) of charged thermoresponsive copolymers. These developments can be used as design rules for the development of polymer-based soft functional materials, where switching, stimuli-response and adaptivity play key roles for function. The developed models were tested successfully either versus the experiments of our partners or versus monomer- and ion-resolved coarse-grained computer simulations devised and conducted by ourselves. Additionally to move more into the chemical specificity of responsive polymers a new temperature-dependent Hamiltonian was developed for the case of polyethylene glycole (PEG) which is a popular polymer in various architectures nowadays for soft material design. Analogous systematic treatments for other responsive and charged polymers in future modeling efforts may lead to a comprehensive set of coarse-grained building blocks for charges responsive copolymers with which possibly industrially relevant materials can be modeled on large scales with large benefit for material design and process optimization.
Publications
- Thermodynamic description of the LCST of charged thermosensitive copolymers. Macromolecules 47, 2096 (2014)
J. Heyda, S. Soll, J. Yuan, and J. Dzubiella
(See online at https://doi.org/10.1021/ma402577h) - Tuning the critical solution temperature of polymers by copolymerization. J. Chem. Phys. 143, 243119 (2015)
B. Schulz, R. Chudoba, J. Heyda, and J. Dzubiella
(See online at https://doi.org/10.1063/1.4934017) - A temperature-dependent implicit solvent model of polyethylene glycole in aqueous solution. J. Chem. Theo. Comp. 13, 6317 (2017)
R. Chudoba, J. Heyda, and J. Dzubiella
(See online at https://doi.org/10.1021/acs.jctc.7b00560) - Beyond the Hofmeister Series: Ion Specific Effects on Proteins and Their Biological Functions. J. Phys. Chem. B 121, 1997 (2017)
H. J., Okur, J. Hladílková, K. Rembert, J. Heyda, J. Dzubiella, P. Cremer, and P. Jungwirth
(See online at https://doi.org/10.1021/acs.jpcb.6b10797)
