Designing materials capable of interfacing with and learning from the body is a major driving force for developing organic mixed ionio-electronic conductors (OMIECs). When integrated into transducing devices, such conductors have enabled on-body computing of biological signals, owing to their better flexibility, stretchability, biocompatibility, low-power consumption, and chemical tunability, compared to their inorganic counterparts. However, OMIECs still suffer from limitations, including poor charge carrier mobility, limited mechanical properties, and low environmental stability, which hinder their application for bioelectronics. If proper design of polymer backbones and sidechains can circumvent some of these restrictions while improving mixed ionic-electronic conductivity, blending organic semiconducting polymers with insulators offers an extra dimension to tune the morphology and electronic properties of the semiconducting polymer. In this work, we developed organic iono-electronic composites (OIECs) with tunable structure and electrochemical properties by blending poly(methyl methacrylate) (PMMA) -of different tacticities and ratios- with a novel OMIEC material (PDPP3T-20gT) made of polar tetraethylene glycol side chains tethered to a backbone of 80% diketopyrrolopyrrole and 20% glycolated thiophene. Electrochemical properties were assessed using transducing electrochemical transistors. High resolution microscopy, X-ray crystallography, and spectroscopy were used to probe polymer-polymer interactions at the nanoscale and investigate morphology changes upon blending. By systematically engineering OIECs structure and properties, and enhance mixed-ionic electronic conduction, we propose a versatile route towards more stable, mechanically compliant, and readily processable functional channel materials, which will facilitate their implementation into transducing devices for on-body computing, smart electronics, and point-of-care monitoring.

Engineering iono-electronic composite materials for high-performance organic electronics

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