The coupling among electron transfer, deformation, screening and binding in electrochemically active macromolecules
Literature Information
Waldemar A. Marmisollé, M. Inés Florit, Dionisio Posadas
Experimental data are presented demonstrating that electrochemically active macromolecules show a coupling among electron transfer, deformation, screening and binding. The work includes dependence of the redox potential of synthetic and natural electrochemically active polymers on the electrolyte pH (electron transfer-binding coupling), the changes in volume during the redox switching of synthetic electrochemically active polymers (deformation-electron transfer coupling) and the changes in the macromolecular conformation during the acid–base titration of polyelectrolytes and proteins (deformation-binding coupling). A simple equilibrium statistical thermodynamic model is presented that allows explaining these couplings effects. The model is based on the assumption that a macromolecule is composed of segments of different length that may bind species present in the external solution and that also contain redox centers that may be oxidized and reduced. The partition function of the system is obtained, and from it the expressions for the redox potentials, the total length and the chemical potential of the bound species are obtained. Simple calculations shows that the model satisfactorily explains the qualitative behavior of the experimental results.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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