Adapting Direct Arylation Polycondensation for Arbitrary Mixed Ionic and Electronic Conductors

Direct arylation polycondensation (DArP) has been developed as a straightforward method for synthesis of conjugated polymers. However, it encounters severe incompatibility with polymer-based organic mixed ionic and electronic conductors (OMIECs) that are essential for neuromorphic engineering and bioelectronics. Herein, we demonstrate trimethyladamantyl-flanked N-heterocyclic carbene (NHC) ligands motivated DArP of OMIECs. Significant steric bulkiness of such ligands shields the catalytic palladium centers against chelating chains in OMIECs. Consequently, adamantyl NHCs modulated DArP provides a general synthetic platform for OMIECs with tailored backbone and side chain variations. Furthermore, this methodology accelerates the exploration of structure-mixed transport correlation as well as optimization of high mobility-volumetric capacitance OMIECs. Through these advancements, we contribute an innovative toolkit to the synthetic repertoire of mixed conducting polymers.