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1. Designing bijels formed by solvent transfer induced phase separation with functional nanoparticles

   https://doi.org/10.1039/C9SM00289H  

   Boakye-Ansah, Stephen ; Schwenger, Matthew S. ; Haase, Martin F. ( April 2019 , Soft Matter)

   Bicontinuous interfacially jammed emulsion gels (bijels) formed via solvent transfer induced phase separation (STrIPS) are new soft materials with potential applications in separations, healthcare, or catalysis. To facilitate their applications, means to fabricate STrIPS bijels with nanoparticles of various surface chemistries are needed. Here, we investigate the formation of STrIPS bijels with nanoparticles of different wettabilities, ranging from partially hydrophobic to extremely hydrophilic. To this end, the surface wettability of silica nanoparticles is tailored by functionalization with ligands bearing either hydrophobic or hydrophilic terminal groups. We show that partially hydrophobic particles with acrylate groups can impart short-term stability to STrIPS bijels on their own. However, to enable long-term stability, the use of cationic surfactants is needed. Partially hydrophobic particles require short chain surfactants for morphological stability while glycerol-functionalized hydrophilic particles require double chain cationic surfactants. Variation of the surfactant concentration results in various STrIPS bijel morphologies with controllable domain sizes. Last, we show that functional groups on the nanoparticles facilitate interfacial cross-linking for the purposes of reinforcing STrIPS bijels. Our research lays the foundation for the use of a wide variety of solid particles, irrespective of their surface wettabilities, to fabricate bijels with potential applications in Pickering interfacial catalysis andmore »as cross-flow microreactors.« less
2. Effect of (3-aminopropyl)triethoxysilane on dissolution of silica nanoparticles synthesized via reverse micro emulsion

   https://doi.org/10.1039/D2NR01190E  

   Kang, Hyunho ; Lee, Jihyeon ; O'Keefe, Tana ; Tuga, Beza ; Hogan Jr., Christopher J. ; Haynes, Christy L. ( June 2022 , Nanoscale)

   Silica nanomaterials have been studied based on their potential applications in a variety of fields, including biomedicine and agriculture. A number of different molecules have been condensed onto silica nanoparticles’ surfaces to present the surface chemistry needed for a given application. Among those molecules, (3-aminopropyl)triethoxysilane (APS) is one of the most commonly applied silanes used for nanoparticle surface functionalization to achieve charge reversal as well as to enable cargo loading. However, the colloidal stability of APS-functionalized silica nanoparticles has not been thoroughly studied, which can be problematic when the high reactivity of amine groups is considered. In this study, four different types of silica nanoparticles with varied location of added APS have been prepared via a reverse micro emulsion process, and their colloidal stability and dissolution behavior have been investigated. Systematic characterization has been accomplished using transmission electron microscopy (TEM), silicomolybdic acid (SMA) spectrophotometric assay, nitrogen adsorption–desorption surface area measurement, and aerosol ion mobility-mass spectrometry to track the nanoparticles’ physical and chemical changes during dissolution. We find that when APS is on the interior of the silica nanoparticle, it facilitates dissolution, but when APS is condensed both on the interior and exterior, only the exterior siloxane bonds experience catalytic hydrolysis,more »and the interior dissolution is dramatically suppressed. The observation and analyses that silica nanoparticles show different hydrolysis behaviors dependent on the location of the functional group will be important in future design of silica nanoparticles for specific biomedical and agricultural applications.« less
3. Scanning force sensing at micrometer distances from a conductive surface with nanospheres in an optical lattice

   https://doi.org/10.1364/AO.457148  

   Montoya, Cris ; Alejandro, Eduardo ; Eom, William ; Grass, Daniel ; Clarisse, Nicolas ; Witherspoon, Apryl ; Geraci, Andrew A. ( January 2022 , Applied Optics)

   The center-of-mass motion of optically trapped dielectric nanoparticles in a vacuum is extremely well decoupled from its environment, making a powerful tool for measurements of feeble subattonewton forces. We demonstrate a method to trap and maneuver nanoparticles in an optical standing wave potential formed by retroreflecting a laser beam from a metallic mirror surface. We can reliably position a ∼ 170 n m diameter silica nanoparticle at distances of a few hundred nanometers to tens of micrometers from the surface of a gold-coated silicon mirror by transferring it from a single-beam tweezer trap into the standing wave potential. We can further measure forces experienced by the particle while scanning the two-dimensional space parallel to the mirror surface, and we find no significant excess force noise in the vicinity of the surface. This method may enable three-dimensional scanning force sensing near surfaces using optically trapped nanoparticles, promising for high-sensitivity scanning force microscopy, tests of the Casimir effect, and tests of the gravitational inverse square law at micrometer scales.
4. Reversible assembly of silica nanoparticles at water–hydrocarbon interfaces controlled by SDS surfactant

   https://doi.org/10.1039/D1NR06807E  

   Mohammed, Sohaib ; Kuzmenko, Ivan ; Gadikota, Greeshma ( December 2021 , Nanoscale)

   Achieving reversible and tunable assembly of silica nanoparticles at liquid–liquid interfaces is vital for a wide range of scientific and technological applications including sustainable subsurface energy applications, catalysis, drug delivery and material synthesis. In this study, we report the mechanisms controlling the assembly of silica nanoparticles (dia. 50 nm and 100 nm) at water–heptane and water–toluene interfaces using sodium dodecyl sulfate (SDS) surfactant with concentrations ranging from 0.001–0.1 wt% using operando ultrasmall/small-angle X-ray scattering, cryogenic scanning electron microscopy imaging and classical molecular dynamics simulations. The results show that the assembly of silica nanoparticles at water–hydrocarbon interfaces can be tuned by controlling the concentrations of SDS. Silica nanoparticles are found to: (a) dominate the interfaces in the absence of interfacial SDS molecules, (b) coexist with SDS at the interfaces at low surfactant concentration of 0.001 wt% and (c) migrate toward the aqueous phase at a high SDS concentration of 0.1 wt%. Energetic analyses suggest that the van der Waals and electrostatic interactions between silica nanoparticles and SDS surfactants increase with SDS concentration. However, the favorable van der Waals and electrostatic interactions between the silica nanoparticles and toluene or heptane decrease with increasing SDS concentration. As a result, the silica nanoparticles migratemore »away from the water–hydrocarbon interface and towards bulk water at higher SDS concentrations. These calibrated investigations reveal the mechanistic basis for tuning silica nanoparticle assembly at complex interfaces.« less
5. Tunable Orientation and Assembly of Polymer-Grafted Nanocubes at Fluid–Fluid Interfaces

   https://doi.org/10.1021/acsnano.1c10416  

   Zhou, Yilong ; Tang, Tsung-Yeh ; Lee, Brian Hyun-jong ; Arya, Gaurav ( April 2022 , ACS Nano)

   Self-assembly of faceted nanoparticles is a promising route for fabricating nanomaterials; however, achieving low-dimensional assemblies of particles with tunable orientations is challenging. Here, we demonstrate that trapping surface-functionalized faceted nanoparticles at fluid–fluid interfaces is a viable approach for controlling particle orientation and facilitating their assembly into unique one- and two-dimensional superstructures. Using molecular dynamics simulations of polymer-grafted nanocubes in a polymer bilayer along with a particle-orientation classification method we developed, we show that the nanocubes can be induced into face-up, edge-up, or vertex-up orientations by tuning the graft density and differences in their miscibility with the two polymer layers. The orientational preference of the nanocubes is found to be governed by an interplay between the interfacial area occluded by the particle, the difference in interactions of the grafts with the two layers, and the stretching and intercalation of grafts at the interface. The resulting orientationally constrained nanocubes are then shown to assemble into a variety of unusual architectures, such as rectilinear strings, close-packed sheets, bilayer ribbons, and perforated sheets, which are difficult to obtain using other assembly methods. Our work thus demonstrates a versatile strategy for assembling freestanding arrays of faceted nanoparticles with possible applications in plasmonics, optics, catalysis, andmore »membranes, where precise control over particle orientation and position is required.« less