Myelin surfactant assemblies shaping the electrodeposition of copper dendrites.

01 April 2024, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Self-organization of inorganic matter enables bottom-up construction of materials with targetted shapes suited to their function. Positioning the building blocks in the growth process involves a well-balanced interplay of reaction and diffusion. Whereas (supra)molecular structures have been used to template such growth processes, we reasoned that molecular assemblies can be employed to actively create concentration gradients which shape the deposition of solid, wire-like structures. The core of our approach comprises the interaction between myelin assemblies that deliver copper(II) ions to the tips of copper dendrites, which in turn grow along the Cu2+-gradient upon electrodeposition. First, we successfully include Cu2+ ions amongst amphiphile bilayers in myelin filaments, which grow from C12E3-based source droplets over air-water interfaces. Second, we characterize the growth of dendritic copper structures upon electrodeposition from a negative electrode at the sub-mM Cu2+ concentrations that are anticipated upon release from the copper loaded myelins. Third, we assess the intricate growth of copper dendrites upon electrodeposition, when combined with copper loaded myelins. The myelins deliver Cu2+ at a negative electrode, feeding copper dendrite growth upon electrodeposition. Intriguingly, the copper dendrites follow the Cu2+ gradient towards the myelins, and grow along them towards the source droplet. We demonstrate the growth of dynamic connections amongst electrodes and surfactant droplets in reconfigurabe setups – featuring a unique interplay between molecular assemblies and inorganic, solid structures. With the growing interest in neuromorphic circuitry, we envision such a self-organizing system opening entirely new pathways for interconnected networks of (semi)conductive wires that are integrated with soft-matter based systems.

Keywords

self-assembly
self-organization
responsive materials
soft matter
gradients
fractal dendrites
electrodeposition
myelins
Marangoni flow
surfactants
amphiphiles

Supplementary materials

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Movie 1
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Optical microscopy recording of CuCl2/C12E3 source droplet deposited on MQ water (MP4).
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Movie 2
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Optical microscopy recordings of copper dendrite growth from working electrodes placed in aqueous CuCl2 solutions (10 µM to 1 mM) over a time period of 20 minutes (MP4).
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Movie 3
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Optical microscopy recordings of copper dendrites growing from the copper working electrode (- 8 V) that interact with the Cu2+-loaded myelins growing from the source on MQ water.
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Movie 4
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Optical microscopy recordings of the interactions of the Cu2+-loaded myelins and the dendrites growing from two different copper electrodes that are consecutively applied as working electrode (-8 V) (MP4).
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Movie 5
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Optical microscopy recordings of multiple connections established amongst a Cu2+-loaded source droplet placed amongst 6 copper electrodes in a hexagonal array. (MP4)
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Movie 6
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Optical microscopy recording of dynamic, reconfigurable connections amongst a Cu2+-loaded source droplet placed amongst 6 gold plated electrodes in a hexagonal array. (MP4)
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Supporting Information
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Additional experimental details, materials and methods, supporting figures and descriptions of supporting movies.
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