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1.
PNAS Nexus ; 3(8): pgae331, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-39211516

RESUMEN

Biological or biomimetic membranes are examples within the larger material class of flexible ultrathin lamellae and contoured fluid sheets that require work or energy to impose bending deformations. Bending elasticity also dictates the interactions and assembly of integrated phases or molecular clusters within fluid lamellae, for instance enabling critical cell functions in biomembranes. More broadly, lamella and other thin fluids that integrate dispersed objects, inclusions, and phases behave as contoured 2D colloidal suspensions governed by elastic interactions. To elucidate the breadth of interactions and assembled patterns accessible through elastic interactions, we consider the bending elasticity-driven assembly of 1-10 µm solid plate-shaped Brownian domains (the 2D colloids), integrated into a fluid phospholipid membrane (the 2D fluid). Here, the fluid membranes of giant unilamellar vesicles, 20-50 µm in diameter, each contain 4-100 monodisperse plate-domains at an overall solid area fraction of 17 ± 3%. Three types of reversible plate arrangements are found: persistent vesicle-encompassing quasi-hexagonal lattices, persistent closely associated chains or concentrated lattices, and a dynamic disordered state. The interdomain distances evidence combined attractive and repulsive elastic interactions up to 10 µm, far exceeding the ranges of physio-chemical interactions. Bending contributions are controlled through membrane slack (excess area) producing, for a fixed composition, a sharp cooperative multibody transition in plate arrangement, while domain size and number contribute intricacy.

2.
Nat Commun ; 15(1): 3442, 2024 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-38658581

RESUMEN

The morphologies of two-dimensional (2D) crystals, nucleated, grown, and integrated within 2D elastic fluids, for instance in giant vesicle membranes, are dictated by an interplay of mechanics, permeability, and thermal contraction. Mitigation of solid strain drives the formation of crystals with vanishing Gaussian curvature (i.e., developable domain shapes) and, correspondingly, enhanced Gaussian curvature in the surrounding 2D fluid. However, upon cooling to grow the crystals, large vesicles sustain greater inflation and tension because their small area-to-volume ratio slows water permeation. As a result, more elaborate shapes, for instance, flowers with bendable but inextensible petals, form on large vesicles despite their more gradual curvature, while small vesicles harbor compact planar crystals. This size dependence runs counter to the known cumulative growth of strain energy of 2D colloidal crystals on rigid spherical templates. This interplay of intra-membrane mechanics and processing points to the scalable production of flexible molecular crystals of controllable complex shape.

3.
Sci Adv ; 7(14)2021 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-33811075

RESUMEN

We demonstrate how manipulating curvature in an elastic fluid lamella enables the reversible relative positioning of flat, rigid, plate-like micrometer-scale inclusions, with spacings from about a micrometer to tens of micrometers. In an experimental model comprising giant unilamellar vesicles containing solid domain pairs coexisting in a fluid membrane, we adjusted vesicle inflation to manipulate membrane curvature and mapped the interdomain separation. A two-dimensional model of the pair potential predicts the salient experimental observations and reveals both attractions and repulsions, producing a potential minimum entirely a result of the solid domain rigidity and bending energy in the fluid membrane. The impact of vesicle inflation on domain separation in vesicles containing two solid domains was qualitatively consistent with observations in vesicles containing many domains. The behavior differs qualitatively from the pure repulsions between fluid membrane domains or interactions between nanoscopic inclusions whose repulsive or attractive character is not switchable.

4.
Beilstein J Nanotechnol ; 8: 2264-2270, 2017.
Artículo en Inglés | MEDLINE | ID: mdl-29181283

RESUMEN

ZnO quantum dots and KNb3O8 nanosheets were synthesized by a two-step hydrothermal method for the photocatalytic reduction of CO2 to methanol where isopropanol is simultaneously oxidized to acetone . The as-prepared photocatalysts were characterized by X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM) and UV-vis absorption spectroscopy (UV-vis). The photocatalytic activity of the materials was evaluated by formation rate of methanol under UV light irradiation at ambient temperature and pressure. The methanol formation rate of pure KNb3O8 nanosheets was found to be 1257.21 µmol/g/h, and after deposition of 2 wt % ZnO quantum dots on the surface of KNb3O8 nanosheets, the methanol production rate was found to increase to 1539.77 µmol/g/h. Thus, the ZnO quantum dots obviously prompted separation of charge carriers, which was explained by a proposed mechanism for this photocatalytic reaction.

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