Controlling the electro-mechanical performance of polypyrrole through 3- and 3,4-methyl substituted copolymers

Conducting polymers such as polypyrrole are biocompatible materials used in bioelectronic applications and microactuators for mechanobiology and soft microrobotics. The materials are commonly electrochemically synthesised from an electrolyte solution comprising pyrrole monomers and a salt, which is incorporated as the counter ion. This electrosynthesis results in polypyrrole forming a three-dimensional network with extensive cross-linking in both the alpha and beta positions, which impacts the electro-mechanical performance. In this study we adopt a 'blocking strategy' to restrict and control cross-linking and chain branching through beta substitution of the monomer to investigate the effect of crosslinking on the electroactive properties. Methyl groups where used as blocking groups to minimise the impact on the pyrrole ring system. Pyrrole, 3- and 3,4-methyl substituted pyrrole monomers were electro-polymerised both as homo-polymers and as a series of co-polymer films. The electroactive performance of the films was characterised by measuring their electrochemical responses and their reversible and non-reversible film thickness changes. This showed that altering the degree of crosslinking through this blocking strategy had a large impact on the reversible and irreversible volume change. These results elaborate the importance of the polymer structure in the actuator performance, an aspect that has hitherto received little attention.