Imine‐Based Polymeric Mixed Ionic–Electronic Conductors Featuring Degradability and Biocompatibility for Transient Bioinspired Electronics

Abstract Degradable features are highly desirable to advance next‐generation organic mixed ionic–electronic conductors (OMIECs) for transient bioinspired artificial intelligence devices. It is highly challenging that OMIECs exhibit excellent mixed ionic‐electronic behavior and show degradability simultaneously. Specially, in OMIECs, doping is often a tradeoff between structural disorder and charge carrier mobilities. Here, we describe a regiochemistry‐driven backbone curvature approach to prepare OMIECs, enabling doped state ordered within efficient ionic‐electronic conduction in organic electrochemical transistors (OECTs) and presenting degradable characteristics. Significantly, i ‐3gTIT shows an outstanding mobility (1.99 cm 2 V −1 s −1 ) and μ C* (302 F V −1 cm −1 s −1 ), and presents higher disorder‐tolerance upon doping and faster degradation behavior than its regioisomer, o ‐3gTIT . Especially, the resulting OECT‐based inverter shows a high voltage gain of 31.6 V V −1 at a low driving voltage of 0.6 V. Moreover, we demonstrate an application of transient OECT, i. e., biodegradable solid‐state electrolyte of OECT‐based artificial synapses. Remarkably, the regiochemistry‐driven film crystallinity modulation enables the conversion from volatile to non‐volatile operation in such synapses. The transient synapse based on i ‐3gTIT achieves over 90 % recognition accuracy for small digit handwritten images, showing potential in security neuromorphic computing. Our work is the first presentation enabling excellent mixed conduction of OMIECs with degradable features for transient bioinspired electronics.