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1. Binding, unbinding and aggregation of crescent-shaped nanoparticles on nanoscale tubular membranes

   https://doi.org/10.1039/D0SM01642J  

   Spangler, Eric J.; Olinger, Alexander D.; Kumar, P. B.; Laradji, Mohamed (January 2021, Soft Matter)

   null (Ed.)

   Using molecular dynamics simulations of a coarse-grained implicit solvent model, we investigate the binding of crescent-shaped nanoparticles (NPs) on tubular lipid membranes. The NPs adhere to the membrane through their concave side. We found that the binding/unbinding transition is first-order, with the threshold binding energy being higher than the unbinding threshold, and the energy barrier between the bound and unbound states at the transition that increases with increasing the NP's arclength L np or curvature mismatch μ = R c / R np , where R c and R np are the radii of curvature of the tubular membrane and the NP, respectively. Furthermore, we found that the threshold binding energy increases with increasing either L np or μ . NPs with curvature larger than that of the tubule ( μ > 1) lie perpendicularly to the tubule's axis. However, for μ smaller than a specific arclength-dependent mismatch μ *, the NPs are tilted with respect to the tubule's axis, with the tilt angle that increases with decreasing μ . We also investigated the self-assembly of the NPs on the tubule at relatively weak adhesion strength and found that for μ > 1 and high values of L np , the NPs self-assemble into linear chains, and lie side-by-side. For μ < μ * and high L np , the NPs also self-assemble into chains, while being tilted with respect to the tubule's axis. 

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2. Preferential interactions of primary amine-terminated quantum dots with membrane domain boundaries and lipid rafts revealed with nanometer resolution

   https://doi.org/10.1039/C9EN00996E  

   Mensch, Arielle C.; Melby, Eric S.; Laudadio, Elizabeth D.; Foreman-Ortiz, Isabel U.; Zhang, Yongqian; Dohnalkova, Alice; Hu, Dehong; Pedersen, Joel A.; Hamers, Robert J.; Orr, Galya (January 2020, Environmental Science: Nano)

   The initial interactions of engineered nanoparticles (NPs) with living cells are governed by physicochemical properties of the NP and the molecular composition and structure of the cell membrane. Eukaryotic cell membranes contain lipid rafts – liquid-ordered nanodomains involved in membrane trafficking and molecular signaling. However, the impact of these membrane structures on cellular interactions of NPs remains unclear. Here we investigate the role of membrane domains in the interactions of primary amine-terminated quantum dots (Qdots) with liquid-ordered domains or lipid rafts in model membranes and intact cells, respectively. Using correlative atomic force and fluorescence microscopy, we found that the Qdots preferentially localized to boundaries between liquid-ordered and liquid-disordered phases in supported bilayers. The Qdots also induced holes at these phase boundaries. Using super resolution fluorescence microscopy (STORM), we found that the Qdots preferentially co-localized with lipid rafts in the membrane of intact trout gill epithelial cells – a model cell type for environmental exposures. Our observations uncovered preferential interactions of amine-terminated Qdots with liquid-ordered domains and their boundaries, possibly due to membrane curvature at phase boundaries creating energetically favorable sites for NP interactions. The preferential interaction of the Qdots with lipid rafts supports their potential internalization via lipid raft-mediated endocytosis and interactions with raft-resident signaling molecules. 

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3. Penetration and preferential binding of charged nanoparticles to mixed lipid monolayers: interplay of lipid packing and charge density

   https://doi.org/10.1039/d0sm01945c  

   Chaudhury, Anurag; Debnath, Koushik; Bu, Wei; Jana, Nikhil R.; Basu, Jaydeep Kumar (February 2021, Soft Matter)

   null (Ed.)

   Designing of nanoparticles (NPs) for biomedical applications or mitigating their cytotoxic effects requires microscopic understanding of their interactions with cell membranes. Such insight is best obtained by studying model biomembranes which, however, need to replicate actual cell membranes, especially their compositional heterogeneity and charge. In this work we have investigated the role of lipid charge density and packing of phase separated Langmuir monolayers in the penetration and phase specificity of charged quantum dot (QD) binding. Using an ordered and anionic charged lipid in combination with uncharged but variable stiffness lipids we demonstrate how the subtle interplay of zwitterionic lipid packing and anionic lipid charge density can affect cationic nanoparticle penetration and phase specific binding. Under identical subphase pH, the membrane with higher anionic charge density displays higher NP penetration. We also observe coalescence of charged lipid rafts floating amidst a more fluidic zwitterionic lipid matrix due to the phase specificity of QD binding. Our results suggest effective strategies which can be used to design NPs for diverse biomedical applications as well as to devise remedial actions against their harmful cytotoxic effects especially against respiratory diseases. 

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4. Improving anti-fouling properties of alumina tubular microfiltration membranes through the use of hydrophilic silica nanoparticles for oil/water separation

   https://doi.org/10.1080/01496395.2023.2259605  

   Ghosh, Anirban; Mahmodi, Ghader; Miranda, Michael; Xie, Songpei; Shaw, Madelyn; Krzmarzick, Mark; Lampert, David J.; Kim, Seok-Jhin; Aichele, Clint P. (September 2023, Separation Science and Technology)

   In this study, hydrophilic silica nanoparticles (Si NPs) were used to modify α-alumina tubular membranes to improve their performance in terms of flux, oil rejection, and anti-fouling properties. Our work focuses on enhancing membrane performance, particularly for difficult applications such as produced water treatment. The prepared membranes were applied for oil-in-water emulsion treatment. After coating hydrophilic Si NPs, the oil contact angle improved from 133.8° to 171.4°. To prevent Si NPs from leaching off the surface of α-alumina tubular membranes, polyvinyl alcohol was used to coat the membranes as a pre-treatment step before Si NP modification. After coating the membrane with Si NPs, the roughness of the membrane surface decreased, likely leading to less fouling. After coating Si NPs, Total Organic Carbon rejection increased from 93.1% for pristine α-alumina tubular membranes to 97.7% for silica-modified membranes because of hydrophilic improvements of the modified membranes. The Si NP coating improved the anti-fouling property of membranes with the flux recovery ratio increasing from 71.3% for pristine α-alumina tubular membranes to 85.9% for silica-modified membranes. Scanning Electron Microscopy, Energy- dispersive X-ray spectroscopy, oil contact angle, and Atomic Force Microscopy characterization tests were done. The tests showed successful Si NPs impregnation and altered wettability. 

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5. Ligand‐Mediated Interaction of Nanoparticles with Lipid Membranes

   https://doi.org/10.1002/mats.202300058  

   Mathew, Sandeep; Laradji, Mohamed; Kumar, P. B. Sunil (December 2023, Macromolecular Theory and Simulations)

   Abstract While many studies are performed on the effect of ligands on the adhesion and endocytosis of NPs, the effects of ligand length and surface density on the NPs' interaction with lipid membranes are poorly investigated. Here, a computational investigation is presented, based on molecular dynamics of a coarse‐grained implicit‐solvent model, of the interaction between ligand‐decorated spherical NPs and lipid membranes. Specifically,the case is considered where the ligands interact attractively with lipid membranes only through their ends. In particular, the effects of ligand grafting density, ligand length, and strength of ligand‐lipid interaction is investigated on the degree of wrapping of the NP by the membrane and on the morphology of the membrane close to the NP. Whereas the degree of wrapping is found to increase with increasing the grafting density for a given interaction strength and ligand length, it decreases with ligand length for a given grafting density and interaction strength. For moderate values of the adhesion strength and long ligands, it is found that the end ligands form long linear clusters, which lead to an anisotropic conformation of the membrane around the NP. For short ligands, the wrapping of the membrane around the NP is almost complete, with the wrapped NP showing a regular faceted structure for high adhesion strength. 

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