RESUMEN

Concentrated ionic aqueous electrolytes possess a diverse array of applications across various fields, particularly in the field of energy storage. Despite extensive examination, the intricate relationships and numerous physical mechanisms underpinning diverse phenomena remain incompletely understood. Molecular dynamics simulations are employed to probe the attributes of aqueous solutions containing LiCl, NaCl, KCl, MgCl2, and CaCl2, spanning various solute fractions. The primary emphasis of the simulations is on unraveling the intricate interplay between these attributes and the underlying physical mechanisms. The configurations of cation-Cl- and Cl--Cl- pairs within these solutions are disclosed. As the solute fraction increases, consistent trends manifest regardless of solute type: (i) the number of hydrogen bonds formed by the hydration water surrounding ions decreases, primarily attributed to the growing presence of counter ions in proximity to the hydration water; (ii) the hydration number of ions exhibits varying trends influenced by multiple factor; and (iii) the diffusion of ions slows down, attributed to the enhanced confinement and rebound of cations and Cl- ions from the surrounding atoms, concurrently coupled with the changes in ion vibration modes. In our analysis, we have, for the first time, clarified the reasons behind the slowing down of the diffusion of the ions with increasing solute fraction. Our research contributes to a better understanding and manipulation of the attributes of ionic aqueous solutions and may help designing high-performance electrolytes.

RESUMEN

The dispersity of nonpolar nanoparticles (NPs) in water/ethanol mixed solvents was studied using molecular dynamics simulations. Based on the rule of "like dissolves like," nonpolar NPs should be dispersed better in a solvent with a lower polarity. As the mole fraction of ethanol in a mixed solvent (R) increases from 0% (pure water) to 100% (pure ethanol), the polarity of the mixed solvent is indicated to decrease monotonically. However, the dispersity of nonpolar NP does not increase monotonically: it first decreases after the addition of a small fraction of ethanol (R < 8.0%) and then markedly increases as R further grows. When there is a small amount of ethanol, the ethanol molecules around aggregated NPs tend to simultaneously make contact with multiple NPs, which can increase the tendency of NP aggregation. Furthermore, with a considerable ethanol ratio, the interaction of the solvent with NPs becomes notably strong, which facilitates the dissolution of NPs. Our findings may help to better understand the mechanism of dispersion of NPs in mixed solvents and may provide a useful precipitation technology for NP production.

RESUMEN

The evaporation of water nanofilms on a solid surface is a widespread and important process in many fields. Herein, we utilize molecular dynamics simulations to demonstrate that the evaporation of a water nanofilm is regulated by applying an alternating electric field (AEF). An AEF at a specific frequency can be resonantly absorbed by the water film. Consequently, the AEF with sufficient strength significantly increases the evaporation rate of the water film (R). In contrast, an AEF of a different frequency and polarization direction decreases R sharply, which is closely related to the strengthened hydrogen bond network and the reduced kinetic energy of the outermost water of the water film. When the maximum amplitude of the AEFs is 0.9 V/nm, which is achievable in a laboratory setting, R spans six orders of magnitude. The effects of applying the AEFs are quite distinct from those of changing the temperature. Notably, the polarization direction of the AEF plays an important role in the water evaporation. To the best of our knowledge, this is the first report on regulating the evaporation rate of a water film, showing that it is possible to use AEFs to tune the properties of nanoscaled water, such as the wettability.

RESUMEN

The structural and dynamic properties of water molecules in a uniformly charged nanopore have been studied using the method of classical molecular dynamics simulation. When confined in an uncharged nanopore with an appropriate radius, water molecules are aligned along the nanopore axis and form a single-file structure with the dipole vectors pointing toward the same end of the nanopore. We demonstrate here that when the nanopore is uniformly charged, the water molecules in the nanopore pack more tightly and the water molecules near the two ends of the nanopore are no longer aligned along the nanopore axis but tend to be aligned perpendicularly to the nanopore axis. The water dipole vectors do not point toward the same nanopore end. When the nanopore is positively charged, the water molecules in the nanopore align with their oxygen atoms pointing to the center of the nanopore. The central water molecule forms an L-defect. However for a negatively charged nanopore, the water molecules in the nanopore take up the opposite orientation. A D-defect is formed at the center of the nanopore. Furthermore, the water molecules in the negatively charged nanopore with moderate atomic partial charges diffuse and transport more quickly than the water molecules in an uncharged nanopore.

RESUMEN

In order to study the dependence of water solubility and hydration behavior of nanoparticles on their surface polarity, we designed polar nanoparticles with varying surface polarity by assigning atomic partial charge to the surface of C60. The water solubility of the nanoparticle is enhanced by several orders of magnitude after the introduction of surface polarity. Nevertheless, when the atomic partial charge grows beyond a certain value (qM), the solubility continuously decreases to the level of nonpolar nanoparticle. It should be noted that such qM is comparable with atomic partial charge of a variety of functional groups. The hydration behaviors of nanoparticles were then studied to investigate the non-monotonic dependence of solubility on the surface polarity. The interaction between the polar nanoparticle and the hydration water is stronger than the nonpolar counterpart, which should facilitate the dissolution of the nanoparticles. On the other hand, the surface polarity also reduces the interaction of hydration water with the other water molecules and enhances the interaction between the nanoparticles which may hinder their dispersion. Besides, the introduction of surface polarity disturbs and even rearranges the hydration structure of nonpolar nanoparticle. Interestingly, the polar nanoparticle with less ordered hydration structure tends to have higher water solubility.

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RESUMEN

The transport properties of water through a nanochannel influenced by the direction of an external electric field has been investigated by using molecular dynamics simulations. Water molecules flow unidirectionally across the nanochannel under a uniform external electric field without an osmotic pressure. It is found that the direction of the external field plays an important role in the interactions and dipole orientations of water molecules in the nanochannel, accordingly changing the net water flux dramatically. Most importantly, a critical angle (θC) between the external field and the nanochannel axis is found. The average net water flux increases as θ increases for θ≤θC but decreases sharply to a near-zero value for a further increase of θ. The maximum value of the average net water flux is 7.33 times as high as the value when the electric field is along the nanochannel axis. Our findings are of great practical importance for nanomolecular engineering, which provide a possible strategy for designing novel controllable water nanopumps.

RESUMEN

BtuCD-BtuF from Escherichia coli is a binding protein-dependent adenosine triphosphate (ATP)-binding cassette (ABC) transporter system that uses the energy of ATP hydrolysis to transmit vitamin B12 across cellular membranes. Experimental studies have showed that during the transport cycle, the transporter undergoes conformational transitions between the "inward-facing" and "outward-facing" states, which results in the open-closed motions of the cytoplasmic gate of the transport channel. The opening-closing of the channel gate play critical roles for the function of the transporter, which enables the substrate vitamin B12 to be translocated into the cell. In the present work, the extent of opening of the cytoplasmic gate was chosen as a function-related internal coordinate. Then the mean-square fluctuation of the internal coordinate, as well as the cross-correlation between the displacement of the internal coordinate and the movement of each residue in the protein, were calculated based on the normal mode analysis of the elastic network model to analyze the function-related motions encoded in the structure of the system. In addition, the key residues important for the functional motions of the transporter were predicted by using a perturbation method. In order to facilitate the calculations, the internal coordinate was introduced as one of the axes of the coordinate space and the conventional Cartesian coordinate space was transformed into the internal/Cartesian space with linear approximation. All the calculations were carried out in this internal/Cartesian space. Our method can successfully identify the functional motions and key residues for the transporter BtuCD-BtuF, which are well consistent with the experimental observations.

Asunto(s)

RESUMEN

A solution processed MoO3/PEDOT:PSS bilayer structure is used as the hole transporting layer to improve the efficiency and stability of planar heterojunction perovskite solar cells. Increased hole extraction efficiency and restrained erosion of ITO by PEDOT: PSS are demonstrated in the optimized device due to the incorporation of an MoO3 layer.

RESUMEN

We demonstrate high-efficient white organic light-emitting diodes (WOLEDs) based on triplet multiple quantum well (MQW) structure and focus on the influence on WOLEDs through employing different potential barrier materials to form type-I and type-II MQWs, respectively. It is found that type-I MQW structure WOLEDs based on 1,3,5-tris(N-phenyl-benzimidazol-2-yl)benzene as potential barrier layer (PBL) offers high electroluminescent (EL) performance. That is to say, maximum current efficiency and power efficiency are achieved at about 1,000 cd/m2 with 16.4 cd/A and 8.3 lm/W, which increase by 53.3% and 50.9% over traditional three-layer structure WOLEDs, respectively, and a maximum luminance of 17,700 cd/m2 is earned simultaneously. The achievement of high EL performance would be attributed to uniform distribution and better confinement of carriers within the emitting layer (EML). However, when 4,7-diphenyl-1,10-phenanthroline or 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline is used as PBL to form type-II MQW structure, poor EL performance is obtained. We attribute that to improper energy level alignment between the interface of EML/PBL, which leads to incomplete confinement and low recombination efficiency of carriers, a more detailed mechanism was argued.

RESUMEN

White light is emitted by an organic light-emitting diode by inserting two blend layers of m-MTDATA:Al(DBM)(3) and TPD:Bphen between an m-MTDATA hole-transporting layer and a Bphen electron-transporting layer, where m-MTDATA, TPD, Al(DBM)(3), and Bphen are 4,4('),4('')-tris[methylpheny(phenyl)amino]-triphenylamine, N,N(')-bis(3-methylphenyl)-N,N(')-diphenylbenzidine, tris(dibenzoyl methane)-aluminum, and 4,7-diphenyl-1,10-phenanthroline molecules, respectively. The white-light spectrum consists of four broad bands that arise from blue-emitting TPD/Bphen, green-emitting m-MTDATA/Bphen, orange-emitting TPD/Al(DBM)(3), and red-emitting m-MTDATA/Al(DBM)(3) exciplexes, respectively, and strongly overlap at 400-760 nm. Any monomer emission is not generated. A high-color rendering index of 94.1, Commission Internationale de l'Eclairage-1931(x,y) coordinates of (0.33, 0.35), and correlated color temperature of 5477 K were obtained at 10 V. Discussion is given for the formation mechanism of the four exciplexes.

RESUMEN

We demonstrate a nondoped white organic light-emitting diode in which the blue, green, and red emissions are generated from 4,4(')-bis(2,2(')-diphenylvinyl)-1,1(')-biphenyl, tris(8-hydroxyquinoline)aluminum, and a submonolayer of 4-(dicyanomethylene)-2-t-butyl-6-(1,1,7,7- tetramethyl-julolidyl 9-enyl)-4H-pyran layers, respectively. A thin layer of N,N(')-diphenyl-N,N(')-bis(1-naphthyl)(1,1(')-benzidine)-4,4(')-diamine (NPB), which differed from the traditional hole-transporting layer, was introduced into the device. The thickness of this thin NPB layer was changed to tune the chromaticity and optimize the white color quality. The white device with a 3 nm chromaticity-tuning NPB layer gives the Commission Internationale de l'Eclairage-1931 xy coordinate of (0.327, 0.336), a color rendering index of 90.2, a maximum luminance of 19,096 cd/m(2), and a maximum current efficiency of 4.12 cd/A. The electroluminescence mechanism of the white device was also discussed.