Proton‐Conducting Hierarchical Composite Hydrogels Producing First Soft Memcapacitors with Switchable Memory

Abstract Perpetual exigency for environment friendly clean energy and powerful soft electronics has elevated the research on hydrogels in past two decades. Hydrogels are the amplifiers of material properties using manipulation in structure–property relationship via simple, economic yet effective routes. Herein, a set of composite and hybrid hydrogels are developed by hierarchical assembling of clay nanosheets and surfactant micelles those divulge the first example of memcapacitor gels and offer exceptional proton conductivity (1.66–4.34 × 10 –2 S cm −1 ) as a gel material. Further, Congo red, Eosin Y, and Orange G are used to hybridize one of the composites to achieve three hybrid hydrogels. Such hybridization is found to regulate the memristive function selectively from the coupled effect of memcapacitance from the composite. The composite hydrogel highlights its volatile memory with encouraging robustness under environmental conditions, established through various current–voltage ( I – V ) experiments. The electrochemical behaviors including the high proton conductivity are realized from impedance measurements. Material characterizations, experimental results, and in silico optimized structures rationalize composite/hybrid network formation, capacitive/memristive responses, and enhanced proton conduction in the fabricated composite superstructures. Proposed structural models demonstrate two orthogonally oriented structural encryptions to be accountable for the expressed bifunctionality in the hierarchically designed superstructures.