Fuel‐Driven π‐Conjugated Superstructures to Form Transient Conductive Hydrogels

Tsironi, Ifigeneia; Maleszka, Jarek A.; Kriebisch, Brigitte A. K.; Wilson‐Kovacs, Robert S.; Acevedo, Orlando; O'Leary, Shamus Loren; Watt, John Daniel; Boekhoven, Job; Olivier, Jean‐Hubert

doi:10.1002/anie.202417109

Title: Fuel‐Driven π‐Conjugated Superstructures to Form Transient Conductive Hydrogels

Journal Article · 21 October 2024 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202417109 · OSTI ID:2478641

^[1];

^[1]; Kriebisch, Brigitte A. K. ^[2]; Wilson‐Kovacs, Robert S. ^[3];

^[3]; O'Leary, Shamus Loren ^[4];

^[4];

^[2];

^[1]

University of Miami, Coral Gables, FL (United States); The University of New Mexico, Albuquerque, NM (United States)
Technical University of Munich, Garching (Germany)
University of Miami, Coral Gables, FL (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Despite advances in creating dissipative materials with transient properties, such as hydrogels and active droplets, their application remains confined to temporal changes in structural properties. Developing out-of-equilibrium materials whose electronic functions are parameterized by a chemical reaction cycle is challenging. Yet, this class of materials is required to construct biomimetic materials. In contrast to traditional chemical reaction cycles that exploit molecularly dissolved building blocks at thermodynamic equilibrium, we show that fiber structures derived from reactive naphthalene diimide (NDI) building blocks can be used as resting states to form far-from-equilibrium conductive hydrogels after the addition of chemical fuels. Upon fueling the NDI-derived fibers, a dual-component activation and deactivation pathway is deduced by kinetic analysis and is absent when using a molecularly dissolved resting state. Investigating the solid-state morphologies of the structures formed throughout the fuel-driven reaction cycle using cryo-EM reveals that the resting thermodynamic fibers evolve to transient thicker fibrils and layered superstructures. We show that the transient redox-active hydrogels exhibit a nearly threefold increase in electrical conductivity upon fuel consumption before reverting to their original value over hours. In conclusion, these far-from-equilibrium materials are potential candidates in applications such as programmable biorobotics and chemical computing.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); Excellence Strategy and the European Research Council

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2478641

Report Number(s):: LA-UR--24-32229

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 5 Vol. 64; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Fuel‐Driven π‐Conjugated Superstructures to Form Transient Conductive Hydrogels

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