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Spontaneous formation of a self-healing carbon nanoskin at the liquid-liquid interface.

ABSTRACT: Biological membranes exhibit the ability to self-repair and dynamically change their shape while remaining impermeable. Yet, these defining features are difficult to reconcile with mechanical robustness. Here, we report on the spontaneous formation of a carbon nanoskin at the oil-water interface that uniquely combines self-healing attributes with high stiffness. Upon the diffusion-controlled self-assembly of a reactive molecular surfactant at the interface, a solid elastic membrane forms within seconds and evolves into a continuous carbon monolayer with a thickness of a few nanometers. This nanoskin has a stiffness typical for a 2D carbon material with an elastic modulus in bending of more than 40-100 GPa; while brittle, it shows the ability to self-heal upon rupture, can be reversibly reshaped, and sustains complex shapes. We anticipate such an unusual 2D carbon nanomaterial to inspire novel approaches towards the formation of synthetic cells with rigid shells, additive manufacturing of composites, and compartmentalization in industrial catalysis.

SUBMITTER: Bomal E

PROVIDER: S-EPMC9399178 | biostudies-literature | 2022 Aug

REPOSITORIES: biostudies-literature

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Spontaneous formation of a self-healing carbon nanoskin at the liquid-liquid interface.

Bomal Enzo E Grandgeorge Paul P Yeo Reuben J RJ Candau Nicolas N Reis Pedro M PM Frauenrath Holger H

Nature communications 20220823 1

Biological membranes exhibit the ability to self-repair and dynamically change their shape while remaining impermeable. Yet, these defining features are difficult to reconcile with mechanical robustness. Here, we report on the spontaneous formation of a carbon nanoskin at the oil-water interface that uniquely combines self-healing attributes with high stiffness. Upon the diffusion-controlled self-assembly of a reactive molecular surfactant at the interface, a solid elastic membrane forms within ...[more]

PMID: 35999197

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Project description:Quantitatively understanding the self-assembly of amphiphilic macromolecules at liquid-liquid interfaces is a fundamental scientific concern due to its relevance to a broad range of applications including bottom-up nanopatterning, protein encapsulation, oil recovery, drug delivery, and other technologies. Elucidating the mechanisms that drive assembly of amphiphilic macromolecules at liquid-liquid interfaces is challenging due to the combination of hydrophobic, hydrophilic, and Coulomb interactions, which require consideration of the dielectric mismatch, solvation effects, ionic correlations, and entropic factors. Here we investigate the self-assembly of a model block copolymer with various charge fractions at the chloroform-water interface. We analyze the adsorption and conformation of poly(styrene)-block-poly(2-vinylpyridine) (PS-b-P2VP) and of the homopolymer poly(2-vinylpyridine) (P2VP) with varying charge fraction, which is controlled via a quaternization reaction and distributed randomly along the backbone. Interfacial tension measurements show that the polymer adsorption increases only marginally at low charge fractions (<5%) but increases more significantly at higher charge fractions for the copolymer, while the corresponding randomly charged P2VP homopolymer analogues display much more sensitivity to the presence of charged groups. Molecular dynamics (MD) simulations of the experimental systems reveal that the diblock copolymer (PS-b-P2VP) interfacial activity could be mediated by the formation of a rich set of complex interfacial copolymer aggregates. Circular domains to elongated stripes are observed in the simulations at the water-chloroform interface as the charge fraction increases. These structures are shown to resemble the spherical and cylindrical helicoid structures observed in bulk chloroform as the charge fraction increases. The self-assembly of charge-containing copolymers is found to be driven by the association of the charged component in the hydrophilic block, with the hydrophobic segments extending away from the hydrophilic cores into the chloroform phase.

Dataset Information

Spontaneous formation of a self-healing carbon nanoskin at the liquid-liquid interface.

Publications

Spontaneous formation of a self-healing carbon nanoskin at the liquid-liquid interface.

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