Electrically fueled active supramolecular materials

26 July 2021, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Fuel-driven dissipative supramolecular assemblies in biology, such as actin filaments and microtubules contribute to the formation of complex, dynamic structures in living organisms and give rise to emergent functions such as motility, homeostasis, self-healing, and camouflage. Several synthetic dissipative supramolecular materials have been created using chemicals or light as fuel, with the goal of furthering our understanding of biological systems and creating synthetic materials that have life-like dynamic properties. However, electrical energy, one of the most common energy sources, has remained mostly unexplored for such purposes. Here we demonstrate the use of electrically fueled dissipative assembly as a new platform for creating active supramolecular materials. Through an electrochemical redox reaction network operating in mild aqueous buffers, a transient and highly active supramolecular assembly based on a redox-sensitive cysteine derivative is achieved by applying an electric potential. The dissipative self-assembly as well as its emergent properties can be spatiotemporally controlled by modulation of electrical signals on patterned microelectrodes. Using electrical energy as a readily available and clean fuel, we are able to create dissipative supramolecular materials rapidly (in seconds to minutes) and repetitively under mild conditions with directional and spatiotemporal control. As electronic signals are the default information carriers in modern technology, the described approach offers a promising opportunity to integrate active materials into electronic devices for bioelectronics applications.

Supplementary materials

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Electrically fueled active supramolecular materials-SI
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This file contains the details of sample preparation, fabrication of bulk electrochemical cell and microelectrode, confocal laser scanning microscopy data, quantitative image analysis, electrochemical impedance spectroscopy, kinetics, rheology, and cryogenic transmission electron microscopy. Including Supplementary Figures 1-17, Supplementary Scheme 1, Supplementary Table 1, and additional references.
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SI Movie 1-Transient self-assembly
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The Movie 1 shows transient assembly of fiber formation by applying an electric potential, followed by dissolution upon removal of the potential.
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SI Movie 2-Active Dynamic Assembly
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The Movie 2 shows highly active, dynamic assembly of the electrically fueled active system.
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SI Movie 3-Realtime DSSIM
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The Movie 3 shows realtime generation of DSSIM curves from image data analysis.
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SI Movie 4-Spatiotemporal Control
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The Movie 4 shows precise spatiotemporal control of the e-fueled dissipative assembly system.
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