Microcavity array supported lipid bilayer models of ganglioside – influenza hemagglutinin<sub>1</sub> binding

Berselli, Guilherme B.; Sarangi, Nirod Kumar; Gimenez, Aurélien V.; Murphy, Paul V.; Keyes, Tia E.

doi:10.1039/d0cc04276e

Cited by 11 publications

(17 citation statements)

References 33 publications

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“…In this experimental setup previously reported by some of us, [25,26] and coined “microcavity supported lipid bilayers” (MSLBs), the lipid bilayer is supported across aqueous‐filled micron‐diameter pore arrays, shown schematically in Figure S17. The lateral mobility of emissive molecules situated in the membranes located above the pores, because of the aqueous interface at both leaflets, was shown to be very similar to that observed in liposomes of the same composition [27,28] . The micron dimensions of the cavities and the good stability of the supported lipid membranes make this model highly amenable to study lateral diffusion by fluorescence correlation spectroscopy [29] .…”

Section: Resultsmentioning

confidence: 58%

“…The lateral mobility of emissive molecules situated in the membranes located above the pores, because of the aqueous interface at both leaflets, was shown to be very similar to that observed in liposomes of the same composition. [ 27 , 28 ] The micron dimensions of the cavities and the good stability of the supported lipid membranes make this model highly amenable to study lateral diffusion by fluorescence correlation spectroscopy. [29] Due to experimental limitations it was not possible to obtain two‐dimensional diffusion data for the ReC 9 and ReC 19 catalysts, so only the ruthenium photosensitisers were probed.…”

Section: Resultsmentioning

confidence: 99%

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Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO₂‐Reducing Photocatalytic Liposomes

Klein

Rodríguez‐Jiménez

Hoefnagel

et al. 2021

Chemistry A European J

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Covalent functionalisation with alkyl tails is a common method for supporting molecular catalysts and photosensitisers onto lipid bilayers, but the influence of the alkyl chain length on the photocatalytic performances of the resulting liposomes is not well understood. In this work, we first prepared a series of rhenium-based CO 2 -reduction catalysts [Re(4, 9, 12, 15, 17, and 19). We then prepared a series of PEGylated DPPC liposomes containing RuC n and ReC n , hereafter noted C n , to perform photocatalytic CO 2 reduction in the presence of sodium ascorbate. The photocatalytic performance of the C n liposomes was found to depend on the alkyl tail length, as the turnover number for CO (TON) was inversely correlated to the alkyl chain length, with a more than fivefold higher CO production (TON = 14.5) for the C 9 liposomes, compared to C 19 (TON = 2.8). Based on immobilisation efficiency quantification, diffusion kinetics, and time-resolved spectroscopy, we identified the main reason for this trend: two types of membranebound RuC n species can be found in the membrane, either deeply buried in the bilayer and diffusing slowly, or less buried with much faster diffusion kinetics. Our data suggest that the higher photocatalytic performance of the C 9 system is due to the higher fraction of the more mobile and less buried molecular species, which leads to enhanced electron transfer kinetics between RuC 9 and ReC 9 .

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Section: Resultsmentioning

confidence: 58%

Section: Resultsmentioning

confidence: 99%

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO₂‐Reducing Photocatalytic Liposomes

Klein

Rodríguez‐Jiménez

Hoefnagel

et al. 2021

Chemistry A European J

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“…Moreover, one could also expect the EE dynamics to be dependent upon membrane‐fluidity, which is a function of the lipid‐composition. [ 60 ] More complex processes such as membrane invagination could be emulated by incorporating receptor (e.g., globotriaosylceramide) in the membrane model.…”

Section: Discussionmentioning

confidence: 99%

A Nanoplasmonic Assay of Oligonucleotide‐Cargo Delivery from Cationic Lipoplexes

Kho

Berselli

Keyes

2021

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A powerful new biophysical model is reported to assay nanocarrier lipid membrane permeability. The approach employs a nanophotonic biophysical membrane model as an assay to study oligonucleotide escape from delivery vector following fusion with endosomal membrane that relies on plasmonic hotspots within the receptor well, below the membrane to follow cargo arrival. Through the combined use of surface enhanced Raman spectroscopy and fluorescence lifetime correlation spectroscopy (FLCS), the model enables identification of a lipoplex‐mediated endosomal‐escape mechanism facilitated by DOTAP‐oligonucleotide interaction that dictates the rate of oligonucleotide release. This work reveals a hitherto unreported release mechanism as a complex multistep interplay between the oligonucleotide cargo and the target membrane, rather than a process based solely on lipid mixing at the fusing site as previously proposed. This substantiates the observations that lipid mixing is not necessarily followed by cargo release. The approach presents a new paradigm for assessment of vector delivery at model membranes that promises to have wide application within the drug delivery design application space. Overall, this plasmonic membrane model offers a potential solution to address persistent challenges in engineering the release mechanism of large therapeutic molecules from their nanocarrier, which is a major bottleneck in intracellular delivery.

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“…MSLBs were prepared across periodic pore arrays prepared in PDMS for the fluorescence correlation study or in gold for electrochemical experiments by PS sphere templating methods previously described. − Briefly, the gold microcavity arrays were prepared by drop casting PS microspheres of 1 μm of diameter followed by gold electroplating, as described in the schematic presented in Figure a. − To obtain a highly packed microcavity array, highly closed packed monolayers of PS microspheres were cast using the gravity-assisted method onto pre-cut rectangles of gold-coated silicon wafers. Then, gold was electrodeposited to the interstitial surface between the PS microspheres by applying a reduction potential (−0.6 V, Ag/AgCl) to the gold array in the presence of a cyanide-free gold solution.…”

Section: Methodsmentioning

confidence: 99%

Robust Photoelectric Biomolecular Switch at a Microcavity-Supported Lipid Bilayer

Berselli

Gimenez

O’Connor

et al. 2021

ACS Appl. Mater. Interfaces

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Biomolecular devices based on photo-responsive proteins have been widely proposed for medical, electrical, and energy storage and production applications. Also, bacteriorhodopsin (bR) has been extensively applied in such prospective devices as a robust photo addressable proton pump. As it is a membrane protein, in principle, it should function most efficiently when reconstituted into a fully fluid lipid bilayer, but in many model membranes, lateral fluidity of the membrane and protein is sacrificed for electrochemical addressability because of the need for an electroactive surface. Here, we reported a biomolecular photoactive device based on light-activated proton pump, bR, reconstituted into highly fluidic microcavity-supported lipid bilayers (MSLBs) on functionalized gold and polydimethylsiloxane cavity array substrates. The integrity of reconstituted bR at the MSLBs along with the lipid bilayer formation was evaluated by fluorescence lifetime correlation spectroscopy, yielding a protein lateral diffusion coefficient that was dependent on the bR concentration and consistent with the Saffman–Delbrück model. The photoelectrical properties of bR-MSLBs were evaluated from the photocurrent signal generated by bR under continuous and transient light illumination. The optimal conditions for a self-sustaining photoelectrical switch were determined in terms of protein concentration, pH, and light switch frequency of activation. Overall, a significant increase in the transient current was observed for lipid bilayers containing approximately 0.3 mol % bR with a measured photo-current of 250 nA/cm 2 . These results demonstrate that the platforms provide an appropriate lipid environment to support the proton pump, enabling its efficient operation. The bR-reconstituted MSLB model serves both as a platform to study the protein in a highly addressable biomimetic environment and as a demonstration of reconstitution of seven-helix receptors into MSLBs, opening the prospect of reconstitution of related membrane proteins including G-protein-coupled receptors on these versatile biomimetic substrates.

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Microcavity array supported lipid bilayer models of ganglioside – influenza hemagglutinin₁ binding

Abstract: Microcavity supported Lipid Bilayers (MSLBs) are demonstrated as versatile platforms for modelling unit steps in viral-membrane interactions. The binding of influenza receptor (HA1) to membranes containing different glycosphingolipid receptors was...

Cited by 11 publications

References 33 publications

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO₂‐Reducing Photocatalytic Liposomes

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO₂‐Reducing Photocatalytic Liposomes

A Nanoplasmonic Assay of Oligonucleotide‐Cargo Delivery from Cationic Lipoplexes

Robust Photoelectric Biomolecular Switch at a Microcavity-Supported Lipid Bilayer

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Microcavity array supported lipid bilayer models of ganglioside – influenza hemagglutinin1 binding

Abstract: Microcavity supported Lipid Bilayers (MSLBs) are demonstrated as versatile platforms for modelling unit steps in viral-membrane interactions. The binding of influenza receptor (HA1) to membranes containing different glycosphingolipid receptors was...

Cited by 11 publications

References 33 publications

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO2‐Reducing Photocatalytic Liposomes

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO2‐Reducing Photocatalytic Liposomes

A Nanoplasmonic Assay of Oligonucleotide‐Cargo Delivery from Cationic Lipoplexes

Robust Photoelectric Biomolecular Switch at a Microcavity-Supported Lipid Bilayer

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Product

Resources

About

Microcavity array supported lipid bilayer models of ganglioside – influenza hemagglutinin₁ binding

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO₂‐Reducing Photocatalytic Liposomes

Shorter Alkyl Chains Enhance Molecular Diffusion and Electron Transfer Kinetics between Photosensitisers and Catalysts in CO₂‐Reducing Photocatalytic Liposomes