Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.209
Publication date: 7th February 2022
Conjugated polymers with polar side chains are capable of mixed electronic and ionic conduction, making them attractive candidates for electrodes in electrochemical devices. Their electrochemical and redox properties can be tuned through choice of polymer backbone and side chain [1, 2] while the processible nature of the materials facilitates both manufacture and recycling. When applied as electrodes in electrochemical energy storage devices, conjugated polymer electrodes show excellent charging and discharging rates, high coulometric efficiency and compatibility with simple salt-water electrolytes, whilst specific capacity and stability in ambient environments need to be improved [3]. In this work, we investigate the impact of the of side-chain and backbone structure on the redox properties, charging rate, specific capacity, mass uptake and cycling stability of the electrodes. We show that small changes of the side chain composition can significantly influence the degree of water uptake (and thereby the mechanical stability of the electrodes), the redox-stability of the materials in aqueous electrolytes, and the electrodes’ specific capacity. We use molecular dynamics simulations to understand how the side chain structure controls the internal microstructure of the polymer electrode and its response to water and ion uptake. We also explore differences in the mechanisms of charging in n and p-type polymers. Finally, we consider different strategies for enhancing specific capacity. The findings can help to develop chemical designs for improved conjugated polymer electrodes for aqueous environments.
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