journal article·2025-07Open access

Supramolecular Conductive Hydrogels With Homogeneous Ionic and Electronic Transport

Stephen J.K. O'Neill, Minoru Ashizawa, Alan M. McLean, Ruben Ruiz‐Mateos Serrano, Tokihiko Shimura, Masakazu Agetsuma, Motosuke Tsutsumi, Tomomi Nemoto, Christopher D. J. Parmenter, Jade A. McCune, George G. Malliaras, Naoji Matsuhisa, Oren A. Scherman

Advanced Materials· Volume 37· Issue 26

Abstract

Abstract Mechanically resilient hydrogels with ion‐electron mixed transport properties effectively bridge biology with electronics. An ideal bioelectronic interface can be realized through introducing electronically conductive polymers into supramolecular hydrogels. However, inhomogeneous morphologies of conducting polymers, such as poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), have limited mechanical properties and ion‐electron interactions. Here, supramolecular conductive hydrogels that possess homogeneous ionic and electronic transport are achieved. The materials demonstrate high toughness (620 kJ m −3 ), stretchability (>1000%), softness (10.5 kPa), and conductivity (5.8 S cm −1 ), which surpasses commonly used inhomogeneous PEDOT:PSS‐based hydrogels. The homogeneous network leads to higher charge injection capacitance and lower skin impedance compared to commercial electrodes or commonly used inhomogeneous PEDOT:PSS conducting networks. This significant advance arises from the homogeneous incorporation of the hydrophilic self‐doped conducting polymer S‐PEDOT, which has polymerized within a supramolecular polymer network template mediated by high‐binding affinity host‐guest crosslinks. Furthermore, the compatibility of S‐PEDOT with hydrophilic secondary networks enables the realization of fully dryable and reswellable electronic devices, facilitating reusability and improving their ease of handling. It is anticipated that achieving such material architectures will offer a promising new direction in future synthesis and implementation of conductive hydrogels in the field of bioelectronics.
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Research context

OpenAlex topics: Conducting polymers and applications · Advanced Sensor and Energy Harvesting Materials · Supercapacitor Materials and Fabrication

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Melville Laboratory for Polymer Synthesis, Yusuf Hamied Department of Chemistry University of Cambridge Lensfield Road Cambridge CB2 1EW UK

Department of Materials Science and Engineering Tokyo Institute of Technology 2‐12‐1 Ookayama, Meguro‐ku Tokyo 152‐8552 Japan

Electrical Engineering Division, Department of Engineering University of Cambridge 9 JJ Thomson Ave Cambridge CB3 0FA UK

Research Center for Advanced Science and Technology The University of Tokyo 4‐6‐1 Komaba, Meguro‐ku Tokyo 153‐8505 Japan

Electronics and Electrical Engineering, Faculty of Science and Engineering Keio University 3‐14‐1 Hiyoshi, Kohoku‐ku, Yokohama Kanagawa 223‐8522 Japan

Institute of Industrial Science The University of Tokyo 4‐6‐1 Komaba, Meguro‐ku Tokyo 153‐8505 Japan

Division of Homeostatic Development National Institute for Physiological Sciences 38 Nishigohnaka Myodaiji‐cho, Okazaki Aichi 444‐8585 Japan

Quantum Regenerative and Biomedical Engineering Team, Institute for Quantum Life Science National Institutes for Quantum Science and Technology (QST) Anagawa 4‐9‐1, Chiba Inage‐ku Chiba 263‐8555 Japan

Biophotonics Research Group, Exploratory Research Center on Life and Living Systems National Institutes of Natural Sciences Okazaki Aichi 444‐8787 Japan

Research Division of Biophotonics, National Institute for Physiological Sciences National Institutes of Natural Sciences Okazaki Aichi 444‐8787 Japan

Nottingham Nanoscale and Microscale Research Centre University of Nottingham University Park Nottingham NG7 2RD UK

Funding

Engineering and Physical Sciences Research Council · Japan Society for the Promotion of Science · European Research Council

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