Experimental and simulation study of self-assembly and adsorption of glycerol monooleate in n-dodecane with varying water content onto iron oxide.

The self-assembly and surface adsorption of glycerol monooleate (GMO) in n-dodecane are studied using a combination of experimental and molecular dynamics simulation techniques. The self-assembly of GMO to form reverse micelles, with and without added water, is studied using small-angle neutron scattering and simulations. A large-scale simulation is also used to investigate the self-assembly kinetics. GMO adsorption onto iron oxide is studied using depletion isotherms, neutron reflectometry, and simulations. The adsorbed amounts of GMO, and any added water, are determined experimentally, and the structures of the adsorbed films are investigated using reflectometry. Detailed fitting and analysis of the reflectometry measurements are presented, taking into account various factors such as surface roughness, and the presence of impurities. The reflectometry measurements are complemented by molecular dynamics simulations, and good consistency between both approaches is demonstrated by direct comparison of measured and simulated reflectivity and scattering length density profiles. The results of this analysis are that in dry systems, GMO adsorbs as self-assembled reverse micelles with some molecules adsorbing directly to the surface through the polar head groups, while in wet systems, the GMO is adsorbed onto a thin layer of water. Only at high surface coverage is some water trapped inside a reverse-micelle structure; at lower surface coverages, the GMO molecules associate primarily with the water layer, rather than self-assemble.

α-Synuclein fibril and synaptic vesicle interactions lead to vesicle destruction and increased lipid-associated fibril uptake into iPSC-derived neurons.

Monomeric alpha-synuclein (aSyn) is a well characterised protein that importantly binds to lipids. aSyn monomers assemble into amyloid fibrils which are localised to lipids and organelles in insoluble structures found in Parkinson's disease patient's brains. Previous work to address pathological aSyn-lipid interactions has focused on using synthetic lipid membranes, which lack the complexity of physiological lipid membranes. Here, we use physiological membranes in the form of synaptic vesicles (SV) isolated from rodent brain to demonstrate that lipid-associated aSyn fibrils are more easily taken up into iPSC-derived cortical i3Neurons. Lipid-associated aSyn fibril characterisation reveals that SV lipids are an integrated part of the fibrils and while their fibril morphology differs from aSyn fibrils alone, the core fibril structure remains the same, suggesting the lipids lead to the increase in fibril uptake. Furthermore, SV enhance the aggregation rate of aSyn, yet increasing the SV:aSyn ratio causes a reduction in aggregation propensity. We finally show that aSyn fibrils disintegrate SV, whereas aSyn monomers cause clustering of SV using small angle neutron scattering and high-resolution imaging. Disease burden on neurons may be impacted by an increased uptake of lipid-associated aSyn which could enhance stress and pathology, which in turn may have fatal consequences for neurons.

Decreased Water Mobility Contributes To Increased α-Synuclein Aggregation.

The solvation shell is essential for the folding and function of proteins, but how it contributes to protein misfolding and aggregation has still to be elucidated. We show that the mobility of solvation shell H2 O molecules influences the aggregation rate of the amyloid protein α-synuclein (αSyn), a protein associated with Parkinson's disease. When the mobility of H2 O within the solvation shell is reduced by the presence of NaCl, αSyn aggregation rate increases. Conversely, in the presence CsI the mobility of the solvation shell is increased and αSyn aggregation is reduced. Changing the solvent from H2 O to D2 O leads to increased aggregation rates, indicating a solvent driven effect. We show the increased aggregation rate is not directly due to a change in the structural conformations of αSyn, it is also influenced by a reduction in both the H2 O mobility and αSyn mobility. We propose that reduced mobility of αSyn contributes to increased aggregation by promoting intermolecular interactions.

Decreased Water Mobility Contributes To Increased α-Synuclein Aggregation.

The solvation shell is essential for the folding and function of proteins, but how it contributes to protein misfolding and aggregation has still to be elucidated. We show that the mobility of solvation shell H2O molecules influences the aggregation rate of the amyloid protein α-synuclein (αSyn), a protein associated with Parkinson's disease. When the mobility of H2O within the solvation shell is reduced by the presence of NaCl, αSyn aggregation rate increases. Conversely, in the presence CsI the mobility of the solvation shell is increased and αSyn aggregation is reduced. Changing the solvent from H2O to D2O leads to increased aggregation rates, indicating a solvent driven effect. We show the increased aggregation rate is not directly due to a change in the structural conformations of αSyn, it is also influenced by a reduction in both the H2O mobility and αSyn mobility. We propose that reduced mobility of αSyn contributes to increased aggregation by promoting intermolecular interactions.

Optimising correlative super resolution and atomic force microscopies for investigating the cellular cytoskeleton.

Correlative imaging methods can provide greater information for investigations of cellular ultra-structure, with separate analysis methods complementing each other's strengths and covering for deficiencies. Here we present a method for correlative applications of super resolution and atomic force microscopies, optimising the sample preparation for correlative imaging of the cellular cytoskeleton in COS-7 cells. This optimisation determined the order of permeabilisation and fixation, the concentration of Triton X-100 surfactant used and time required for sufficient removal of the cellular membrane while maintaining the microtubule network. Correlative SMLM/AFM imaging revealed the different information that can be obtained through each microscopy. The widths of microtubules and microtubule clusters were determined from both AFM height measurements and Gaussian fitting of SMLM intensity cross sections, these were then compared to determine the orientation of microtubules within larger microtubule bundles. The ordering of microtubules at intersections was determined from the AFM height profiles as each microtubule crosses the other. The combination of both microtubule diameter measurements enabled greater information on their structure to be found than either measurement could individually.

Spontaneous surface adsorption of aqueous graphene oxide by synergy with surfactants.

The spontaneous adsorption of graphene oxide (GO) sheets at the air-water interface is explored using X-ray reflectivity (XRR) measurements. As a pure aqueous dispersion, GO sheets do not spontaneously adsorb at the air-water interface due to their high negative surface potential (-60 mV) and hydrophilic functionality. However, when incorporated with surfactant molecules at optimal ratios and loadings, GO sheets can spontaneously be driven to the surface. It is hypothesised that surfactant molecules experience favourable attractive interactions with the surfaces of GO sheets, resulting in co-assembly that serves to render the sheets surface active. The GO/surfactant composites then collectively adsorb at the air-water interface, with XRR analysis suggesting an interfacial structure comprising surfactant tailgroups in air and GO/surfactant headgroups in water for a combined thickness of 30-40 Å, depending on the surfactant used. Addition of too much surfactant appears to inhibit GO surface adsorption by saturating the interface, and low loadings of GO/surfactant composites (even at optimal ratios) do not show significant adsorption indicating a partitioning effect. Lastly, surfactant chemistry is also a key factor dictating adsorption capacity of GO. The zwitterionic surfactant oleyl amidopropyl betaine causes marked increases in GO surface activity even at very low concentrations (≤0.2 mM), whereas non-ionic surfactants such as Triton X-100 and hexaethyleneglycol monododecyl ether require higher concentrations (ca. 1 mM) in order to impart spontaneous adsorption of the sheets. Anionic surfactants do not enhance GO surface activity presumably due to like-charge repulsions that prevent co-assembly. This work provides useful insight into the synergy between GO sheets and molecular amphiphiles in aqueous systems for enhancing the surface activity of GO, and can be used to inform system formulation for developing water-friendly, surface active composites based around atomically thin materials.

Preparation of Multicore Colloidosomes: Nanoparticle-Assembled Capsules with Adjustable Size, Internal Structure, and Functionalities for Oil Encapsulation.

Colloidosomes, also known as Pickering emulsion capsules, have attracted attention for encapsulation of hydrophilic and hydrophobic actives. However, current preparation methods are limited to single core structures and require the use of modified/engineered nanoparticles for forming the shell. Here, we report a fast, simple, and versatile method for producing multi-oil core silica colloidosomes via salt-driven assembly of purely hydrophilic commercial nanoparticles dispersed within an oil-in-water-in-oil (O/W/O) double emulsion template. The internal structure and overall diameter of the capsules can be adjusted by altering the primary and secondary emulsification conditions. With this approach, 7-35 µm diameter multicore colloidosomes containing 0.9-4.2 µm large oil cores were produced. The capsules can easily be functionalized depending on the type of nanoparticles used in the preparation process. Here, metal oxide nanoparticles, such as Fe3O4, TiO2, and ZnO, were successfully incorporated within the structure, conferring specific functional properties (i.e., magnetism and photocatalysis) to the final microcapsules. These capsules can also be ruptured by using ultrasound, enabling easy access to the internal core environments. Therefore, we believe this work offers a promising approach for producing multicore colloidosomes with adjustable structure and functionalities for the encapsulation of hydrophobic actives.

Towards a neutron and X-ray reflectometry environment for the study of solid-liquid interfaces under shear.

A novel neutron and X-ray reflectometry sample environment is presented for the study of surface-active molecules at solid-liquid interfaces under shear. Neutron reflectometry was successfully used to characterise the iron oxide-dodecane interface at a shear rate of [Formula: see text] [Formula: see text] using a combination of conventional reflectometry theory coupled with the summation of reflected intensities to describe reflectivity from thicker films. Additionally, the structure adopted by glycerol monooleate (GMO), an Organic Friction Modifier, when adsorbed at the iron oxide-dodecane interface at a shear rate of [Formula: see text] [Formula: see text] was studied. It was found that GMO forms a surface layer that appears unaltered by the effect of shear, where the thickness of the GMO layer was found to be [Formula: see text] Å under direct shear at [Formula: see text] [Formula: see text] and [Formula: see text] Å when not directly under shear. Finally, a model to analyse X-ray reflectometry data collected with the sample environment is also described and applied to data collected at [Formula: see text] [Formula: see text].

Self-assembly of TiO2/Fe3O4/SiO2 microbeads: A green approach to produce magnetic photocatalysts.

HYPOTHESIS: A green approach for producing magnetic photocatalysts via direct agglomeration of commercial nanoparticles in emulsion is shown. Aggregation is attributed to charge screening by salt addition which reduces stabilising repulsive forces between particles, and different nanoparticles (TiO2, Fe3O4 and SiO2) serve to imbue the final agglomerates with desired adsorption, photodegradation and magnetic properties. EXPERIMENT: Titania doped magnetic silica microbeads (TiO2/Fe3O4/SiO2) were produced at room temperature by CaCl2-induced aggregation of nanoparticles in a reverse emulsion template. The beads were characterized using optical microscopy, SEM, STEM, EDX and zeta potential measurements. The adsorption and photocatalytic properties of the system as well as its reusability were investigated using Rhodamine B and Methylene Blue as model pollutants. RESULTS: Magnetically responsive beads approximately 3-9 µm in diameter incorporating SiO2, TiO2 and Fe3O4 nanoparticles were produced. Adsorption and photodegradation properties of the beads were confirmed by bleaching solutions of Rhodamine B, Methylene Blue as well as mixtures of both dyes. Reusability of the beads after magnetic separation was demonstrated, exhibiting a dye removal efficiency greater than 93% per cycle for three consecutive cycles of UV-light irradiation. This method is simpler than conventional sol-gel methods and offers a green and easy to implement approach for producing structured functional materials.

Spontaneous Self-Assembly of Thermoresponsive Vesicles Using a Zwitterionic and an Anionic Surfactant.

Spontaneous formation of vesicles from the self-assembly of two specific surfactants, one zwitterionic (oleyl amidopropyl betaine, OAPB) and the other anionic (Aerosol-OT, AOT), is explored in water using small-angle scattering techniques. Two factors were found to be critical in the formation of vesicles: surfactant ratio, as AOT concentrations less than equimolar with OAPB result in cylindrical micelles or mixtures of micellar structures, and salt concentration, whereby increasing the amount of NaCl promotes vesicle formation by reducing headgroup repulsions. Small-angle neutron scattering measurements reveal that the vesicles are approximately 30-40 nm in diameter, depending on sample composition. Small-angle X-ray scattering measurements suggest preferential partitioning of OAPB molecules on the vesicle inner layer to support vesicular packing. Heating the vesicles to physiological temperature (37 °C) causes them to collapse into smaller ellipsoidal micelles (2-3 nm), with higher salt concentrations (≥10 mM) inhibiting this transition. These aggregates could serve as responsive carriers for loading or unloading of aqueous cargoes such as drugs and pharmaceuticals, with temperature changes serving as a simple release/uptake mechanism.

Tuning the structure, thermal stability and rheological properties of liquid crystal phases via the addition of silica nanoparticles.

The effects of adding silica nanoparticles of varying size and surface chemistry to a liquid crystal system were analysed using small-angle scattering and polarising light microscopy, with varying temperature and applied shear. It was found that nanoparticles aggregate at domain boundaries, causing a reduction in average liquid crystal domain size. These particles can inhibit phase transitions that occur at specific temperatures, ascribed to aggregates posing a kinetic barrier to rearrangement required for phase transitions. Nanoparticles can also promote the existence of specific phases, such as a deswollen hexagonal mesophase for the system studied here, suggested to be caused by silica aggregates 'templating' new phases. These findings have important implications for the application of such systems in biotechnology, and particularly the ability to completely inhibit a phase change at low temperature suggests the potential for mechanistic insight into new methods of cryopreservation.

Worm-like micelles and vesicles formed by alkyl-oligo(ethylene glycol)-glycoside carbohydrate surfactants: The effect of precisely tuned amphiphilicity on aggregate packing.

Carbohydrates are appealing non-ionic surfactant head-groups as they are naturally abundant, generally biocompatible and biodegradable, and readily functionalized. Recent work has produced a promising molecular candidate for the formation of viscoelastic worm-like micellar solutions: a tri(ethylene glycol)-linked oleyl-ß-D-glucoside surfactant (GlcC18:1) exhibited near ideal Maxwell behavior at low concentrations (2.9 wt%) without additives at room temperature. Here, fourteen surfactants have been synthesized with structural variations based around GlcC18:1. Each contain an oligo(ethylene glycol) linker of varying length (2, 3, 4, 6 EO units) between a carbohydrate head-group (glucose, galactose, mannose, maltose, lactose, cellobiose) and a cis-unsaturated alkyl tail-group (oleyl, linoleyl, erucyl). The aqueous adsorption kinetics and self-assembly of these surfactants was explored using tensiometry and small-angle neutron scattering (SANS), respectively. With SANS we observed the formation of worm-like micelles for four surfactants, and vesicles for two surfactants which exhibited behavior similar to insoluble lipids. We also observed temperature-induced micellar elongation due to dehydration of the oligo(ethylene glycol) linker, resulting in a further three surfactants forming worm-like micelles at 50 °C. Worm-like micellar fluids were further characterized using rheology to reveal two surfactants with vastly superior viscoelastic properties compared to GlcC18:1, with >2 orders of magnitude increase in viscosity and >3 orders of magnitude increase in stress relaxation time. These results provide insight into structure-function relationships for non-ionic surfactants and demonstrate a class of designed amphiphiles with a special propensity for forming viscoelastic worm-like micellar solutions at low concentrations.

Rich liquid crystal phase behavior of novel alkyl-tri(ethylene glycol)-glucoside carbohydrate surfactants.

Carbohydrates are appealing non-ionic surfactant head-groups as they are naturally abundant, generally biocompatible and biodegradable, and readily functionalized. Herein, we explore the phase behavior of seven novel carbohydrate-based surfactants (CBS) containing a tri-ethylene glycol (TEG) linker between a glucose head-group and alkyl tail-group, with linear saturated (C8-18) and cis-unsaturated (C18:1) alkyl chains. At high aqueous concentrations, these glycolipid-like surfactants transition into a variety of lyotropic liquid crystalline phases following an expected concentration phase sequence: hexagonal (H1) → bicontinuous cubic (V1) → lamellar (Lα). Using polarizing light microscopy (PLM), a binary (surfactant-water) phase diagram for each surfactant was constructed across a temperature range (25-80 °C) revealing thermotropic behavior and a broadening of liquid crystal phase regions with increasing alkyl chain length. There was also a significant difference between saturated and unsaturated alkyl chains, due to the cis-unsaturated 'statistical bend' lowering the melting point. Small-angle X-ray scattering (SAXS) measurements were performed to characterize the liquid crystal phases, identifying highly-ordered p6m,Ia3d, and Lα crystallographic space-groups with up to 7 resolved Bragg peaks, likely due to the highly anisometric nature of the TEG-linked surfactants. The phases were shown to be more numerous and exhibited greater thermal-stability compared to well-characterized alkyl glucoside surfactants lacking an oligoethylene spacer in the literature. Finally, the characteristic dimensions of each phase were determined to enable visualization of the internal microstructures, providing insight into the impact of molecular shape and the distribution of hydro-philicity/phobicity on the formation and stability of liquid crystalline mesophases.

The effects of small molecule organic additives on the self-assembly and rheology of betaine wormlike micellar fluids.

A model zwitterionic surfactant, oleyl amidopropyl betaine (OAPB), that spontaneously forms viscoelastic wormlike micelles in aqueous solution is mixed with a variety of structurally diverse organic additives. By systematically varying the nature of these additives, insight into the effects of their aromaticity and polarity on the bulk assembly and fluid behaviour of these micelles is gained by the complementary use of small-angle neutron scattering and viscosity measurements. Inclusion of non-polar additives causes the wormlike aggregates to transition into microemulsions above a critical additive concentration; the precise partitioning within the micelle is determined using contrast variation. Alternatively, polar additives do not appear to cause evolution from the wormlike structure, but instead influence the fluid rheology, with some serving to significantly increase viscosity above that of the pure surfactant solution. Addition of these molecules is accompanied by an increase in fluid viscosity when the oxygenated group of the additive is resonance stabilised or acidic. This effect is thought to be a result of surfactant-additive synergism, in which charge screening of the surfactant head-groups causes stronger attractions between molecules, increasing the scission energy of the micelles (i.e. reducing their ability to break apart and reform). Further doping of acidic additives past a critical concentration causes phase separation of the wormlike mixtures. According to ultra-small-angle neutron scattering measurements, the incorporation of all additives (polar or non-polar, aromatic or non-aromatic) results in the formation of 'branched' wormlike networks. These findings emphasise the significant impact of impurities or additives on the properties of aqueous wormlike micellar systems formed by zwitterionic surfactants, and could also inform selection of solutes for controlling fluid rheology.

Wormlike micelle formation of novel alkyl-tri(ethylene glycol)-glucoside carbohydrate surfactants: Structure-function relationships and rheology.

Carbohydrates are appealing non-ionic surfactant head-groups as they are naturally abundant, generally biocompatible and biodegradable, and readily functionalized. Here, seven novel carbohydrate based surfactants (CBS) have been synthesized that contain a tri-ethylene glycol (TEG) linker between a glucose head-group and alkyl tail-group, with linear saturated (C8-18) and unsaturated (C18:1) alkyl chains. The aqueous adsorption and self-assembly of these surfactants was explored using tensiometry and small- and ultra-small-angle neutron scattering (SANS and USANS). With SANS we observed elongation from spherical to cylindrical micelles with increasing alkyl chain length. C16 and C18 chains exhibited pronounced Krafft points, yet formed worm-like micelles as single components upon heating to 43 and 48 °C respectively. The introduction of mono-unsaturation in the form of a C18:1 chain reduced the Krafft point and gave a surfactant that produced worm-like micelles in water without additives at room temperature. We also observed micellar elongation for C12 and C14 chains at 50 °C due to dehydration of the TEG linker. The room temperature worm-like micelles were further characterized using rheo-SANS and rheology, revealing the C18:1 surfactant to exhibit near ideal Maxwell behavior at low concentrations (2.9 wt.%). These results provide insight into structure-function relationships for CBS, and demonstrate a promising molecular candidate for the formation of viscoelastic worm-like micellar solutions.

Bulk properties of aqueous graphene oxide and reduced graphene oxide with surfactants and polymers: adsorption and stability.

A diverse range of molecular surfactants and polymers have been incorporated into aqueous graphene oxide (GO) and reduced graphene oxide (rGO) dispersions in order to understand the complex relationship between surface chemistry, surface forces and interfacial thermodynamics of these materials with typical amphiphiles. Surfactant additives were systematically varied in terms of their charge and hydrophobicity to reveal important structure-function relationships affecting adsorption and interaction with GO and rGO surfaces. Small-angle (and ultra small-angle) neutron scattering was employed to examine and monitor the interactions and self-assembly in each system. Charge was found to be the overriding factor driving adsorption, as cationic surfactants very readily adsorbed to both GO and rGO, whereas anionic surfactants gave little to no evidence of adsorption despite possessing hydrophobic tail-groups. Molecules of neutral charge such as nonionic and zwitterionic surfactants as well as neutral polymers also showed strong affinities for GO and rGO, indicating that dispersion and dipole (induction polarisation) interactions also play a significant role in adsorption with these materials. Modelling the neutron data revealed in many cases a q-2 slope in the low q and ultra low q regions, indicating that scattering was occurring from large, flat surfaces (lamellae or bilayers), suggesting an effective flattening of the sheets in dispersion. The results presented thus help to form a roadmap for the behaviour of GO and rGO with surfactants and polymers, relevant to adsorption, stabilisation, formulation and coating in aqueous environments as adsorbent and functional materials.

Structural and rheological changes of lamellar liquid crystals as a result of compositional changes and added silica nanoparticles.

Lamellar liquid crystals comprising oil, water and surfactant(s) were formulated and analysed in order to examine how these materials responded to the inclusion of inorganic nanoparticles, in terms of their structural and rheological characteristics. Lamellar phases were formed from mixtures of water, para-xylene and Triton X-100, and analysis was performed via small-angle neutron scattering (SANS), polarising light microscopy (PLM), and amplitude and viscosity sweeps. The partial replacement of Triton X-100 with oleic acid appeared to cause an increase in bilayer thickness, attributed to less efficient packing of the different molecules. Addition of oleic acid also appeared to cause both a loss in lamellar repeat ordering, attributed to heterogeneity of the bilayers, and a rise in long range order, potentially caused by the stiffer bilayers. Adding silica nanoparticles of different size and surface chemistry caused a stiffening of the samples at the expense of a longer-range lamellar repeat order. This strengthening is attributed to aggregation at the domain boundaries, and it was found that hydrophobic particles tended to form stronger aggregates while for larger particles (20 nm as opposed to 10 nm) aggregation was apparently reversible. These results give a more comprehensive understanding of how to reliably control the structural and rheological properties of lamellar liquid crystals, and emphasise the importance of the size and surface chemistry of any inclusions, for applications in cosmetics, drug delivery, and microfluidics.

Self-Assembly of Long-Chain Betaine Surfactants: Effect of Tailgroup Structure on Wormlike Micelle Formation.

Long-chain amidopropyl betaines are known for their ability to self-assemble into viscoelastic wormlike micellar structures. Here, we explore the effect of tailgroup molecular architecture on this process, comparing five molecules, each with C18 chains but different levels of unsaturation and branching. The surfactants are synthesized from stearic, oleic, linoleic, linolenic, and isostearic acids. The self-assembly of these molecules in aqueous solutions is explored using small- and ultra-small-angle neutron scattering (SANS and USANS). It is seen that optimum wormlike micelle formation is achieved for the oleic-chained surfactant, and the alignment of self-assembled structures is further explored using rheo-SANS. The more highly unsaturated molecules form rodlike micelles, whereas the stearic-tailed molecule shows a pronounced Krafft point and the isostearic-chained surfactant is entirely water-insoluble. These results demonstrate the critical importance of tailgroup geometry on surfactant properties and self-assembly for this industrially important class of surfactants.

Synthesis and Characterization of Graphene Oxide-Polystyrene Composite Capsules with Aqueous Cargo via a Water-Oil-Water Multiple Emulsion Templating Route.

Graphene oxide/polystyrene (GO/PS) nanocomposite capsules containing a two-compartment cargo have been successfully fabricated using a Pickering emulsion strategy. Highly purified GO sheets with typically micrometer-scale lateral dimensions and amphiphilic characteristics were prepared from the oxidation reaction of graphite with concomitant exfoliation of the graphite structure. These GO sheets were employed as a stabilizer for oil-in-water emulsions where the oil phase comprised toluene or olive oil. The stability and morphology of the emulsions were extensively studied as a function of different parameters including GO concentration, aqueous phase pH, ultrasonication time, effects of added electrolytes and stability to dilution. In selected conditions, the olive oil emulsions showed spontaneous formation of multiple w/o/w emulsions with high stability, whereas toluene formed simple o/w emulsions of lower overall stability. Olive oil emulsions were therefore used to prepare capsules templated from emulsion droplets by surrounding the oil phase with a GO/PS shell. The GO sheets, emulsions and composite capsules were characterized using a variety of physical and spectroscopic techniques in order to unravel the interactions responsible for capsule formation. The ability of the capsules to control the release of a model active agent in the form of a hydrophilic dye was explored, and release kinetics were monitored using UV-visible spectroscopy to obtain rate parameters. The composite capsules showed promising sustained release properties, with release rates 11× lower than the precursor GO-stabilized multiple emulsion droplets.

Structural Evolution of Wormlike Micellar Fluids Formed by Erucyl Amidopropyl Betaine with Oil, Salts, and Surfactants.

Solutions of extended, flexible cylindrical micelles, often known as wormlike micelles, have great potential as the base for viscoelastic complex fluids in oil recovery, drilling, and lubrication. Here, we study the morphology and nanostructural characteristics of a model wormlike micellar fluid formed from erucyl amidopropyl betaine (EAPB) in water as a function of a diverse range of additives relevant to complex fluid formulation. The wormlike micellar dispersions are extremely oleo-responsive, with even as little as 0.1% hydrocarbon oil causing a significant disruption of the network and a decrease in zero-shear viscosity of around 100-fold. Simple salts have little effect on the local structure of the wormlike micelles but result in the formation of fractal networks at larger length scales, whereas even tiny amounts of small organic species such as phenol can cause unexpected phase transitions. When forming mixtures with other surfactants, a vast array of self-assembled structures are formed, from spheres to ellipsoids, lamellae, and vesicles, offering the ultimate sensitivity in designing formulations with specific nanostructural characteristics.