Single-walled carbon nanotubes have many potential beneficial uses, with additional applications constantly being investigated. Their unique properties, however, create a potential concern regarding toxicity, not only in humans and animals but also in plants. To help develop protocols to determine the effects of nanotubes on plants, we conducted a pilot study on the effects of functionalized and nonfunctionalized single-walled carbon nanotubes on root elongation of six crop species (cabbage, carrot, cucumber, lettuce, onion, and tomato) routinely used in phytotoxicity testing. Nanotubes were functionalized with poly-3-aminobenzenesulfonic acid. Root growth was measured at 0, 24, and 48 h following exposure. Scanning-electron microscopy was used to evaluate potential uptake of carbon nanotubes and to observe the interaction of nanotubes with the root surface. In general, nonfunctionalized carbon nanotubes affected root length more than functionalized nanotubes. Nonfunctionalized nanotubes inhibited root elongation in tomato and enhanced root elongation in onion and cucumber. Functionalized nanotubes inhibited root elongation in lettuce. Cabbage and carrots were not affected by either form of nanotubes. Effects observed following exposure to carbon nanotubes tended to be more pronounced at 24 h than at 48 h. Microscopy images showed the presence of nanotube sheets on the root surfaces, but no visible uptake of nanotubes was observed.
We have studied assembly at air-water and liquid-liquid interfaces with an emphasis on systems containing both surfactants and nanoparticles. Anionic surfactants, sodium dodecyl sulfate (SDS) and non-ionic surfactants, Triton X-100 and tetraethylene glycol alkyl ethers (C(8)E(4), C(12)E(4) and C(14)E(4)), effectively decrease the surface tension of air-water interfaces. The inclusion of negatively charged hydrophilic silica nanoparticles (diameters of approximately 13 nm) increases the efficiency of the SDS molecules but does not alter the performance of the non-ionic surfactants. The former is likely due to the repulsive Coulomb interactions between the SDS molecules and nanoparticles which promote the surfactant adsorption at air-water interfaces. For systems involving trichloroethylene (TCE)-water interfaces, the SDS and Triton X-100 surfactants effectively decrease the interfacial tensions and the nanoparticle effects are similar compared to those involving air-water interfaces. Interestingly, the C(12)E(4) and C(14)E(4) molecules, with or without the presence of nanoparticles, fail to decrease the TCE-water interfacial tensions. Our molecular dynamics simulations have suggested that the tetraethylene glycol alkyl ether molecules tend to disperse in the TCE phase rather than adsorb at the TCE-water interfaces.
We have performed molecular dynamics (MD) simulations to investigate self-assembly at water–trichloroethylene (TCE) interfaces with the emphasis on systems containing modified hydrocarbon nanoparticles (1.2 nm in diameter) and sodium dodecyl sulfate (SDS) surfactants. The nanoparticles and surfactants were first distributed randomly in the water phase. The MD simulations have clearly shown the progress of migration and final equilibrium of the SDS molecules at the water–TCE interfaces with the nanoparticles either at or in the vicinity of the interfaces. One unique feature is the ‘attachment’ of surfactant molecules to the nanoparticle clusters in the water phase followed by the ‘detachment’ at the water–TCE interfaces. At low concentrations of surfactants, the surfactants and nanoparticles co-equilibrate at the interfaces. However, the surfactants, at high concentrations, competitively dominate the interfaces and deplete nanoparticles away from the interfaces. The interfacial properties, such as interfacial thickness and interfacial tension, are significantly influenced by the presence of the surfactants, but not the nanoparticles. The order of the surfactants at the interfaces increases with increasing surfactant concentration, but is independent of nanoparticle concentration. Finally, the simulation has shown that surfactants can aggregate along the water–TCE interfaces, with and without the presence of nanoparticles.
We have used molecular dynamics simulations to investigate the in situ self-assembly of modified hydrocarbon nanoparticles (mean diameter of 1.2 nm) at a water-trichloroethylene (TCE) interface. The nanoparticles were first distributed randomly in the water phase. The MD simulation shows the in situ formation of nanoparticle clusters and the migration of both single particles and clusters from the water phase to the trichloroethylene phase, possibly due to the hydrophobic nature of the nanoparticles. Eventually, the single nanoparticles or clusters equilibrate at the water-TCE interface, and the surrounding liquid molecules pack randomly when in contact with the nanoparticle surfaces. In addition, the simulations show that the water-TCE interfacial thickness analyzed from density profiles is influenced by the presence of nanoparticles either near or in contact with the interface but is independent of the number of nanoparticles present. The nanoparticles, water molecules, and TCE molecules all exhibit diffusion anisotropy.
The driving force for the adsorption of nanoparticles (5-10 nm) at the oil-water interface can be small and is particularly sensitive to the surface chemistry of the particles. Here we show that the interfacial assembly of 5 and 10 nm diameter gold nanoparticles functionalized with stoichiometric ion-pairs is reversible and can be tuned with the solution pH. We also show that at the interface the nanoparticles form a reflective layer with a mirror-like reflectance. Using titration we demonstrate that the mechanism for particle desorption from the interface is the electrostatic repulsion between the nanoparticles, likely due to pH-dependent adsorption of hydroxide ions. By controlling electrostatic repulsion we can control both the extent of adsorption at the interface and the separation between particles within the interfacial film. As such, we demonstrate two avenues to reversibly control the optical properties of the fluid interface: (1) increase the pH of the aqueous solution to desorb particles from the interface, and (2) decrease the ionic strength in the aqueous phase to increase the spacing of the nanoparticles at the oil-water interface.
Using cyclic voltammetry, we studied the reductive desorption of a series of low-density self-assembled monolayers (LD-SAMs) made from mercaptohexadecanoic acid (MHA). Desorption experiments indicate that LD-SAMs are significantly less stable than a full MHA monolayer. All three LD-SAMs investigated presented a broad desorption peak in the region between −1.0 and −0.8 V vs SCE, which is in contrast to the single peak with a narrow distribution at −1.11 V observed for the full MHA monolayer. Upon backfilling the LD-SAM with a shorter-chain thiol (mercaptohexanol), the desorption of the mixed monolayer displayed a single peak, indicative of a well-mixed monolayer. Our results show that LD-SAMs are promising candidates for mixed monolayers and suggest that the broad desorption peak observed for LD-SAMs might arise due to adsorption at different binding sites.
The shape and motion of drops on surfaces is governed by the balance between the driving and the pinning forces. Here we demonstrate control over the motion of droplets on an inclined surface by exerting control over the contact angle hysteresis. The external modulation of contact angle hysteresis is achieved through a voltage-induced local molecular reorganization within the surface film at the solid-liquid interface. We show that tuning contact angle hysteresis alone is sufficient to direct and deform drops when subjected to a constant external driving force, here gravity, in the absence of a pre-defined surface energy gradient or pattern. We also show that the observed stretching and contraction of the drops mimic the motion of an inchworm. Such reversible manipulation of the pinning forces could be an attractive means to direct drops, especially with the dominance of surface forces at micro-/nanoscale.
We have studied the dynamics of nanoparticles at polydimethylsiloxane (PDMS) oil-water interfaces using molecular dynamics (MD) simulations. The diffusion of nanoparticles in pure water and low-viscosity PDMS oil is found to be reasonably consistent with the prediction by the Stokes-Einstein equation. In addition, we have calculated the shear moduli and viscosities of bulk oil and water, as well as oil-water interfaces from single nanoparticle tracking and demonstrated the potential of probing nanorheology from an MD simulation approach. Surprisingly, we found that the lateral diffusion of nanoparticles as well as apparent interfacial nanorheology at the PDMS oil (low viscosity)-water interface are independent of the position of the nanoparticle at the interface.
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