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- Falciani, Gabriele, et al.
(författare)
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Design and testing of a device for the characterization of gas transfer through soap films and measurement protocol based on color matching
- 2023
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Ingår i: International Communications in Heat and Mass Transfer. - : Elsevier. - 0735-1933 .- 1879-0178. ; 149
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Tidskriftsartikel (refereegranskat)abstract
- Soap films are interesting for their potential utilization as soft, self-assembled, self-healing and possibly recyclable membranes. The intrinsic possibility of tuning their properties, such as e.g. surface and bulk elasticity or permeability, via tailored chemistry makes them flexible enough for a wide range of physical-chemical applications. Here we introduce a novel device that can serve as a research platform for the detailed experimental characterization of the soap film permeability to gases. The design and manufacturing of the novel platform are discussed, along with a sample characterization protocol based on a color-matching procedure for dioxygen diffusion through typical soap films. The experimental data is compared with the results obtained from a numerical model, specifically developed for the problem, and good agreement is found. In perspective, the proposed platform can serve for the precise characterization of gas transfer properties of soap films made from different surfactant mixtures and in the presence of different gases.
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- Kaul, Nidhi, et al.
(författare)
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Realizing Symmetry-Breaking Architectures in Soap Films
- 2024
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Ingår i: Physical Review Letters. - : American Physical Society. - 0031-9007 .- 1079-7114. ; 132:2
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Tidskriftsartikel (refereegranskat)abstract
- We show here that soap films-typically expected to host symmetric molecular arrangements-can be constructed with differing opposite surfaces, breaking their symmetry, and making them reminiscent of functional biological motifs found in nature. Using fluorescent molecular probes as dopants on different sides of the film, resonance energy transfer could be employed to confirm the lack of symmetry, which was found to persist on timescales of several minutes. Further, a theoretical analysis of the main transport phenomena involved yielded good agreement with the experimental observations.
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- Pannwitz, Andrea, et al.
(författare)
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Roadmap towards solar fuel synthesis at the water interface of liposome membranes dagger
- 2021
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry. - 0306-0012 .- 1460-4744. ; 50:8, s. 4833-4855
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Forskningsöversikt (refereegranskat)abstract
- Artificial photosynthesis has experienced rapid developments aimed at producing photocatalytic systems for the synthesis of chemical energy carriers. Conceptual advances of solar fuel systems have been inspired by improved understanding of natural photosynthesis and its key operational principles: (a) light harvesting, (b) charge separation, (c) directional proton and electron transport between reaction centres and across membranes, (d) water oxidation and (e) proton or CO2 reduction catalysis. Recently, there has been a surge of bio-inspired photosynthetic assemblies that use liposomes as nanocompartments to confine reaction spaces and enable vectorial charge transport across membranes. This approach, already investigated in the 1980s, offers in principle a promising platform for solar fuel synthesis. However, the fundamental principles governing the supramolecular assemblies of lipids and photoactive surfactant-like molecules in membranes, are intricate, and mastering membrane-supported photochemistry requires thorough understanding of the science behind liposomes. In this review, we provide an overview of approaches and considerations to construct a (semi)artificial liposome for solar fuel production. Key features to consider for the use of liposomes in solar fuel synthesis are highlighted, including the understanding of the orientation and binding of different components along the membrane, the controlled electron transport between the reaction centres, and the generation of proton gradients as driving force. Together with a list of experimental techniques for the characterisation of photoactive liposomes, this article provides the reader with a roadmap towards photocatalytic fuel production at the interface of lipid membranes and aqueous media.
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- Rodriguez-Jimenez, Santiago, et al.
(författare)
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Self-Assembled Liposomes Enhance Electron Transfer for Efficient Photocatalytic CO2 Reduction
- 2022
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 144:21, s. 9399-9412
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Tidskriftsartikel (refereegranskat)abstract
- Light-driven conversion of CO2 to chemicals provides a sustainable alternative to fossil fuels, but homogeneous systems are typically limited by cross reactivity between different redox half reactions and inefficient charge separation. Herein, we present the bioinspired development of amphiphilic photosensitizer and catalyst pairs that self-assemble in lipid membranes to overcome some of these limitations and enable photocatalytic CO2 reduction in liposomes using precious metal-free catalysts. Using sodium ascorbate as a sacrificial electron source, a membrane-anchored alkylated cobalt porphyrin demonstrates higher catalytic CO production (1456 vs 312 turnovers) and selectivity (77 vs 11%) compared to its watersoluble nonalkylated counterpart. Time-resolved and steady-state spectroscopy revealed that self-assembly facilitates this performance enhancement by enabling a charge-separation state lifetime increase of up to two orders of magnitude in the dye while allowing for a ninefold faster electron transfer to the catalyst. Spectroelectrochemistry and density functional theory calculations of the alkylated Co porphyrin catalyst support a four-electron-charging mechanism that activates the catalyst prior to catalysis, together with key catalytic intermediates. Our molecular liposome system therefore benefits from membrane immobilization and provides a versatile and efficient platform for photocatalysis.
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