Interaction Of Water Molecules Research Articles

Development of a ReaxFF reactive force field for ternary phosphate-based bioactive glasses.

Phosphate-based glasses (PBGs) in the CaO-Na2O-P2O5 system have diverse applications as biomaterials due to their unique dissolution properties. A reactive force field (ReaxFF) has been developed to simulate these materials at the atomic level. The ReaxFF parameters of PBGs, including the interaction between phosphorus and calcium atoms, have been developed using a published code based on genetic algorithms. The training data, including the atomic charges, atomic forces, bond and angle parameters, and different differential energies, are chosen and measured from static quantum-mechanical calculations and abinitio molecular dynamics of PBGs. We did different short- and medium-range structural analyses on the bulk simulated PBGs with different compositions to validate the developed potential. Radial and angular distribution functions and coordination numbers of network formers and modifiers, as well as the network connectivity of the glass, are in agreement with experimental and previous simulations using both shell-model classical force fields and abinitio simulated data; for example, the coordination number of phosphorus is 4.0. This successful development of ReaxFF parameters being able to describe the bulk PBGs enables us to work on the dissolution behavior of the glasses, including the interaction of water molecules with PBGs, in future works.

Rotational Dynamics of Water near Osmolytes by Molecular Dynamics Simulations.

The behavior of water molecules around organic molecules has attracted considerable attention as a crucial factor influencing the properties and functions of soft matter and biomolecules. Recently, it has been suggested that the change in protein stability upon the addition of small organic molecules (osmolytes) is dominated by the change in the water dynamics caused by the osmolyte, where the dynamics of not only the directly interacting water molecules but also the long-range hydration layer affect the protein stability. However, the relation between the long-range structure of hydration water in various solutions and the water dynamics remains unclear at the molecular level. We performed density-functional tight-binding molecular dynamics simulations to elucidate the varying rotational dynamics of water molecules in 15 osmolyte solutions. A positive correlation was observed between the rotational relaxation time and our proposed normalized parameter obtained by dividing the number of hydrogen bonds between water molecules by the number of nearest-neighbor water molecules. For the 15 osmolyte solutions, an increase or a decrease in the value of the normalized parameter for the second hydration shell tended to result in water molecules with slow and fast rotational dynamics, respectively, thus illustrating the importance of the second hydration shell for the rotational dynamics of water molecules. Our simulation results are anticipated to advance the current understanding of water dynamics around organic molecules and the long-range structure of water molecules.

Modeling and FE simulation of coupled water diffusion and viscoelasticity in relaxation tests of polyamide 6

AbstractPolyamides can absorb or desorb water from or to their surrounding environment. The impact of this process is significant as water molecules lead locally to a swelling and a coupling of diffusion and deformation behavior. To model these phenomena, a strongly coupled chemo-mechanical (or diffuso-mechanical) model is required, considering both local water concentration and the viscoelastic material behavior of polyamide. In the present work, we derive and apply such a model to polyamide 6. A diffusion equation describing changes in water concentration is coupled to the balance of linear momentum in polyamide 6. The interaction between deformation and concentration is derived from thermodynamic considerations by introducing a free energy consisting of a mechanical and a chemical part. The mechanical part describes a linear viscoelastic model and includes chemical strains due to the presence of water molecules. The chemical part builds upon the theory of Flory and Huggins, that takes into account changes in enthalpy and entropy of mixing due to the interaction of polymer and water molecules. The coupling of deformation to water concentration arises due to a dependency of the water flux on the hydrostatic stress inside the polyamide. We successfully apply the derived model in Finite-Element simulations to predict the drying of polyamide 6 specimens without any coupling to mechanical loads. In addition, we reproduce experimentally obtained data from relaxation measurements, where the drying of polyamide specimens leads to an increase in relaxation modulus.

Toward Modeling the Structure of Electrolytes at Charged Mineral Interfaces Using Classical Density Functional Theory.

The organization of water molecules and ions between charged mineral surfaces determines the stability of colloidal suspensions and the strength of phase-separated particulate gels. In this article, we assemble a density functional that measures the free energy due to the interaction of water molecules and ions in electric double layers. The model accounts for the finite size of the particles using fundamental measure theory, hydrogen-bonding between water molecules using Wertheim's statistical association theory, long-range dispersion interactions using Barker and Henderson's high-temperature expansion, electrostatic correlations using a functionalized mean-spherical approximation, and Coulomb forces through the Poisson equation. These contributions are shown to produce highly correlated structures, aptly rendering the layering of counterions and co-ions at highly charged surfaces and permitting the solvation of ions and surfaces to be measured by a combination of short-range associations and long-ranged attractions. The model is tested in a planar geometry near soft, charged surfaces to reproduce the structure of water near graphene and mica. For mica surfaces, explicitly representing the density of the outer oxygen layer of the exposed silica tetrahedra allows water molecules to hydrogen-bond to the solid. When electrostatic interactions are included, water molecules assume a hybrid character, being accounted for implicitly in the dielectric constant but explicitly otherwise. The disjoining pressure between approaching like-charged surfaces is calculated, demonstrating the model's ability to probe pressure oscillations that arise during the expulsion of ions and water layers from the interfacial gap and predict strong interattractive stresses that form at narrow interfacial spacing when the surface charge is overscreened. This interattractive stress arises not due to in-plane correlations under strong electrostatic coupling but due to the out-of-plane structuring of associating ions and water molecules.

Transferable Water Potentials Using Equivariant Neural Networks.

Machine learning interatomic potentials (MLIPs) have emerged as a technique that promises quantum theory accuracy for reduced cost. It has been proposed [J. Chem. Phys. 2023, 158, 084111] that MLIPs trained on solely liquid water data cannot accurately transfer to the vapor-liquid equilibrium while recovering the many-body decomposition (MBD) analysis of gas-phase water clusters. This suggests that MLIPs do not directly learn the physically correct interactions of water molecules, limiting transferability. In this work, we show that MLIPs using equivariant architecture and trained on 3200 liquid water structures reproduces liquid-phase water properties (e.g., density within 0.003 g/cm3 between 230 and 365 K), vapor-liquid equilibrium properties up to 550 K, the MBD analysis of gas-phase water cluster up to six-body interactions, and the relative energy and the vibrational density of states of ice phases. We show that potentials developed using equivariant MLIPs allow transferability for arbitrary phases of water that remain stable in nanosecond long simulations.

Supramolecular architecture of sodium heterocyclic dithiocarbamate salt: Insights from spectral analysis and bond valence sum characterization

The hydrated sodium salt of 1,2,3,4-tetrahydroquinolinedithiocarbamate (1) has been successfully synthesized and characterized using IR, NMR, and X-ray single crystal analysis. The υC–S and thioureide υC–N bands appeared at 1484 cm−1 and 968 cm−1, respectively, in Na(H2O)3+(thqdtc)– • H2O. The notable NCS2 carbon signal emerged at 212 ppm, credited to unique nitrogen and sulfur-induced deshielding effects. Compound 1 crystallizes in the monoclinic system, P21/c space group, with dimensions a = 14.4297(4) Å, b = 6.1534(2) Å, c = 17.6701(4) Å, β = 108.7340(10)°, V = 1485.83(7) Å3, and Z = 4. The structure of 1 exhibits a supramolecular architecture through secondary interactions, such as weak intermolecular interactions that link the molecules into a linear polymeric chain. The incorporation of heterocyclic rings in the dithiocarbamate ligands leads to the formation of an intriguing supramolecular architecture, as confirmed by BVS analysis results. The BVS value of sodium does not agree well with the formal oxidation state due to the interactions of anions, cations, coordinated and uncoordinated water molecules.

Repulsive Lateral Interaction of Water Molecules at the Initial Stages of Adsorption in Microporous AlPO4-11 According to 27Al NMR and DFT.

Lateral (adsorbate-adsorbate) interactions between adsorbed molecules affect various physical and chemical properties of microporous adsorbents and catalysts, influencing their functional properties. In this work, we studied the hydration of microporous AlPO4-11 aluminophosphate, which has an unusually ordered structure upon adsorption of water vapor, and according to 27Al NMR data, only tetrahedrally or octahedrally coordinated Al sites are present in the AlPO4-11. These 27Al NMR data are consistent with the results of density functional theory (DFT) calculations of hydrated AlPO4-11, which revealed the presence of a strong repulsive lateral interaction at the initial stage of adsorption, suppressing the adsorption of water on neighboring (separated by one -O-P-O- bridge) Al crystallographic sites. As a result, of all the different aluminum sites, only half of the Al1 sites adsorb two water molecules and acquire octahedral coordination.

Effects of Sulfate Ions on Crude Oil Adsorption/Desorption on Carbonate Rocks: Experimental and Molecular Simulations.

In the background of the strong oil wettability and low production by water flooding in carbonate reservoirs, low-salinity water containing sulfate ions can significantly change the surface wettability of carbonate rocks and thus increase the sweeping area; however, the absorption and desorption mechanisms of the oil film in the carbonate rock surface remain unclear. This paper analyzed the wettability alternation of carbonate rocks' surface in pure water and sodium sulfate solution. At the same time, MD (Materials Studio) software was used to simulate the formation process of the oil film and the effect of sulfate ions on the desorption of the oil film on the surface of carbonate rocks. The experimental results showed that sodium sulfate solution could accelerate the rate from oil-wet to water-wet and the final contact angle (49°) was smaller than that in pure water. The simulation results showed that dodecane molecules moved to the surface of calcite to form a double layer of the oil film and that the oil film near the calcite surface had a high-density stable structure under the van der Waals and electrostatic action. The hydrating sulfate ions above the oil film broke through the double oil film to form a water channel mainly under the action of electrostatic force and a hydrogen bond and then adsorbed on the calcite surface. A large number of water molecules moved down the water channel based on a strong hydrogen bonding force and crowded out the oil molecules on the surface of the calcite, resulting in the oil film detachment. This work aims to explain the interaction of oil molecules, water molecules, and SO42- ions at the molecular scale and guide the practical application of low-salinity water flooding in carbonate reservoirs.

Antifreeze Polysaccharides from Wheat Bran: The Structural Characterization and Antifreeze Mechanism.

Exploring a novel natural cryoprotectant and understanding its antifreeze mechanism allows the rational design of future sustainable antifreeze analogues. In this study, various antifreeze polysaccharides were isolated from wheat bran, and the antifreeze activity was comparatively studied in relation to the molecular structure. The antifreeze mechanism was further revealed based on the interactions of polysaccharides and water molecules through dynamic simulation analysis. The antifreeze polysaccharides showed distinct ice recrystallization inhibition activity, and structural analysis suggested that the polysaccharides were arabinoxylan, featuring a xylan backbone with a majority of Araf and minor fractions of Manp, Galp, and Glcp involved in the side chain. The antifreeze arabinoxylan, characterized by lower molecular weight, less branching, and more flexible conformation, could weaken the hydrogen bonding of the surrounding water molecules more evidently, thus retarding the transformation of water molecules into the ordered ice structure.

Light stabilizer-modified hydrocharging melt-blown nonwovens with superior charge stability for air filtration

Particulate matter poses substantial risks to human health, air visibility, climate, and ecological equilibrium. Electret materials are instrumental in air purification and personal protection, as they significantly enhance filtration efficiency without increasing pressure drop. Despite these advantages, developing electret filters with both high filtration efficiency and stable performance under thermal conditions and prolonged storage has proven challenging. In this study, we introduce a novel electret melt-blown filter fabricated through hydrocharging technology supplemented with the light stabilizer UV3346. The interaction of water and air molecules with melt-blown fibers generated abundant positive and negative charges, thereby amplifying the electrostatic attraction effect. Concurrently, UV3346 mitigated the formation of reactive free radicals and minimized charge exchanges, thus enhancing charge storage stability. Owing to the incorporation of UV3346, the UV3346/PP-0.8 melt-blown nonwovens, having a basis weight of 22 g/m2, demonstrated a filtration efficiency of 99.55 %, a low pressure drop of 59.45 Pa, and marginal decrease in filtration efficiency after heat treatment at 130 °C. Notably, the filtration efficiency experienced only a 0.30 % reduction after a two-year storage period, markedly outperforming commercial alternatives. This study is expected to inform future work on high-performance air filtration materials suitable for both air purification and personal protection equipment.

Scalable preparation of flexible heterogeneous graphene oxide structures for high-performance wet power generation

A heterostructured GO-rGO wet power generation device with volt-level potential difference generated by the interaction of water molecules with oxygen groups on graphene oxide and ion-induced diffusion.

Об анизотропии диффузии углеродных нанотрубок в жидкости

This article discusses the methodology and results of molecular dynamics simulation of the diffusion of carbon nanotubes in water. The main goals of this work were to study diffusion longitudinal to an axis of the nanotube and transverse to this axis and determine the velocity autocorrelation functions and diffusion coefficients in these directions. The interaction of water molecules with each other was described by the Lennard-Jones potential, and that of carbon nanotube molecules by the AIREBO potential. The diameters of the nanotubes were 1.15 and 1.44 nanometers, their length varied from 5 to 15 nanometers. The number of water molecules in the simulation cell reached one hundred thousand. It is shown that the nanotube center of mass velocity autocorrelation function in the longitudinal direction decays much more slowly than in the transverse direction. The corresponding values of the diffusion coefficients differ by a factor of 2–4; this diffe¬rence increases with increasing ratio of the nanotube length to its diameter. The directionally averaged diffusion coefficients of flexible nanotubes decrease with increasing nanotube length. Its values exceed the corresponding values for their solid analogues. A nonmonotonic decay of the nanotubes center of mass velocity autocorrelation function was discovered. The characteristic time between the maxima of this function coincides with the period of bending vibrations of the nanotube.

(Invited) Molecular Insights into Water Structure and Proton Transfer at the Interfaces in Bipolar AEM/PEM Membranes

Bipolar membranes (BPMs) are polymeric membranes composed of an acidic proton exchange membrane (PEM) and an alkaline anion exchange membrane (AEM). Bipolar membranes are operated in two different configurations, forward bias and reverse bias, based on the orientation of membranes and electrodes, when the cathode faces the PEM, it is operated in a reverse bias configuration. In reverse bias BPMs facilitates the dissociation of water at the interface of its junction. This unique feature makes it attractive to many industrial applications, including chemical industries, energy conversion and storage, environmental protection, and food processing. It was determined that the rate of water dissociation at the interface of a bipolar membrane increases with the addition of a weak acidic head group material, which acts as the catalyst for the water dissociation reaction and thus referred as the catalyst layer. BPMs have a better ion transport framework because of the amphiphilic nature of all three layers, resulting in well-connected water channels. Hence it is crucial to understand the interaction of water molecules with the functional groups at the molecular level and the morphology at mesoscale to understand the water aggregation and phase separation which helps in the asymmetric transport of proton and hydroxide ions through PEM and AEM respectively.This talk will communicate our efforts to undertake a multiscale approach involving both electronic structure calculations and mesoscale simulations to elucidate: (1) water interaction of water with the headgroups; proton transfer, and (2) connectivity of a TMA AEM, a PFSA PEM, and a phosphonic acid-based catalyst.

Aquatic Functional Liquid Crystals: Design, Functionalization, and Molecular Simulation.

Aquatic functional liquid crystals, which are ordered molecular assemblies that work in water environment, are described in this review. Aquatic functional liquid crystals are liquid-crystalline (LC) materials interacting water molecules or aquatic environment. They include aquatic lyotropic liquid crystals and LC based materials that have aquatic interfaces, for example, nanoporous water treatment membranes that are solids preserving LC order. They can remove ions and viruses with nano- and subnano-porous structures. Columnar, smectic, bicontinuous LC structures are used for fabrication of these 1D, 2D, 3D materials. Design and functionalization of aquatic LC sensors based on aqueous/LC interfaces are also described. The ordering transitions of liquid crystals induced by molecular recognition at the aqueous interfaces provide distinct optical responses. Molecular orientation and dynamic behavior of these aquatic functional LC materials are studied by molecular dynamics simulations. The molecular interactions of LC materials and water are key of these investigations. New insights into aquatic functional LC materials contribute to the fields of environment, healthcare, and biotechnology.

A computational investigation of DMSO/water separation through functionalized GO multilayer nanosheet membrane using molecular dynamics simulation and deep neural network model for membrane performance prediction

In this molecular dynamics (MD) simulation study, the separation of dimethyl sulfoxide (DMSO) from water was investigated using multilayer functionalized graphene oxide (GO) membranes. The GO nanosheets were modified with chemical groups (-F, -H) to alter their properties. The study analyzed the influence of pressure and functional groups on the separation rate. Additionally, a deep neural network (DNN) model was developed to predict membrane behavior under different conditions in water treatment processes. Results revealed that the fluorine-functionalized membrane exhibited higher permeation compared to the hydrogen-functionalized one, with potential of mean force (PMF) analysis indicating higher energy barriers for water molecules passing through the hydrogen-functionalized membrane. The study used density profile, water density map analysis, and radial distribution function (RDF) analysis to understand water and DMSO molecule interactions. The diffusion coefficient of water molecules was also calculated, showing higher diffusion in the fluorine-functionalized system. Overall, the findings suggest that functionalized GO membranes are effective for DMSO-water separation, with the fluorine-functionalized membrane showing superior performance. The DNN model accurately predicts membrane behavior, contributing to the optimization of membrane separation systems.

Diffusion kurtosis imaging and standard diffusion imaging in the magnetic resonance imaging assessment of prostate cancer.

In recent years, magnetic resonance imaging (MRI) has shown excellent results in the study of the prostate gland. MRI has indeed shown to be advantageous in the prostate cancer (PCa) detection, as in guiding targeting biopsy, improving its diagnostic yield. Although current acquisition protocols provide for multiparametric acquisition, recent evidence has shown that biparametric protocols can be non-inferior in PCa detection. Diffusion-weighted imaging (DWI) sequence, in particular, plays a key role, particularly in the peripheral zone which accounts for the larger part of the prostate. High b-values are generally recommended, although with the possibility of obtaining non-Gaussian diffusion effects, which requires a more sophisticated model for the analysis, namely through the diffusion kurtosis imaging (DKI). Purpose of this narrative review was to analyze the current applications and clinical evidence regarding the use of DKI with a main focus on PCa detection, also in comparison with DWI. This narrative review synthesized the findings of literature retrieved from main researches, narrative and systematic reviews, and meta-analyses obtained from PubMed. DKI analyses the non-Gaussian water diffusivity and describe the effect of signal intensity decay related to high b-value through two main metrics (Dapp and Kapp). Differently from DWI-apparent diffusion coefficient (DWI-ADC) which reflects only water restriction outside of cells, DKI metrics are supposed to represent also the direct interaction of water molecules with cell membranes and intracellular compounds. This review describes current evidence on ADC and DKI metrics in clinical imaging, and finally collect the results derived from the main articles focused on DWI and DKI models in detecting PCa. DKI advantages, compared to conventional ADC analysis, still remain controversial. Wider application and greater technical knowledge of DKI, however, may help in proving its intrinsic validity in the field of oncology and therefore in the study of clinically significant PCa. Finally, a deep understanding of DKI is important for radiologists to better understand what Kapp and Dapp mean in the context of different cancer and how these metrics may vary specifically in PCa imaging.

Nanoscale Insights into the Protection of Calcium Silicate Hydrate by Polydimethylsiloxane Coatings in Sulfate Environments: Different Degrees of Polymerization

Calcium silicate hydrate (CSH) plays a crucial role in concrete by controlling its properties and durability. The degradation of CSH often signifies concrete damage. Polydimethylsiloxane (PDMS) is commonly used to protect concrete from sulfate corrosion; however, the comprehensive mechanistic understanding of its protective effects against CSH remains limited. Here, molecular dynamics (MD) simulations were employed to explore atomic-scale interactions between PDMS coatings and CSH in a sulfate-rich environment. Our results reveal that PDMS mitigates sulfate-induced CSH decalcification by forming a positively charged layer, ultimately reducing sulfate bonding by 83.3% compared to the blank group. Molecular structure analysis highlights key hydrogen bonding and calcium–oxygen bonding interactions that are critical for this protection. Higher polymerization stabilizes substrate adsorption, reducing surface diffusion to 33.3% of low-polymerization PDMS, thereby enhancing protection. Additionally, water molecule interactions with the CSH matrix are negatively correlated with the amount of adsorbed sulfate. Simulation results offer valuable insights into the molecular-level dynamic response of the material, contributing to a deeper understanding of the protective mechanisms of PDMS against sulfate-induced CSH degradation in concrete. These findings can guide experimenters and engineers in designing more effective protective coatings for concrete exposed to sulfate-rich environments, thereby laying a foundation for further experimental research and the development of concrete materials with enhanced durability under challenging environmental conditions.

Self-activated superhydrophilic green ZnIn2S4 realizing solar-driven overall water splitting: close-to-unity stability for a full daytime

Engineering an efficient semiconductor to sustainably produce green hydrogen via solar-driven water splitting is one of the cutting-edge strategies for carbon-neutral energy ecosystem. Herein, a superhydrophilic green hollow ZnIn2S4 (gZIS) was fabricated to realize unassisted photocatalytic overall water splitting. The hollow hierarchical framework benefits exposure of intrinsically active facets and activates inert basal planes. The superhydrophilic nature of gZIS promotes intense surface water molecule interactions. The presence of vacancies within gZIS facilitates photon energy utilization and charge transfer. Systematic theoretical computations signify the defect-induced charge redistribution of gZIS enhancing water activation and reducing surface kinetic barriers. Ultimately, the gZIS could drive photocatalytic pure water splitting by retaining close-to-unity stability for a full daytime reaction with performance comparable to other complex sulfide-based materials. This work reports a self-activated, single-component cocatalyst-free gZIS with great exploration value, potentially providing a state-of-the-art design and innovative aperture for efficient solar-driven hydrogen production to achieve carbon-neutrality.

Study of Water Sorption in Methacryl-Based Polyhedral Oligomeric Silsesquioxane (POSS) Dental Composites Using Molecular Dynamics Simulations.

Methacrylate-based polyhedral oligomeric silsesquioxane (POSS) is one of the new composites used as a dental resin. Both monofunctional methacryl isobutyl POSS (MIPOSS) and multifunctional methacryl POSS (MAPOSS) are reported to be possible resins that possess the desired properties for using them as dental resins. Our group's previous comparative study on these two resins showed that the MAPOSS composite has superior mechanical properties compared with the MIPOSS composite. In this article, molecular dynamic simulations (MD simulations) are performed to study the water sorption in these two composites. Water sorption in dental composites can have several effects on the material properties, performance, and longevity of dental restorations. Water sorption in MAPOSS and MIPOSS composites is analyzed by studying the hydrogen bonding, cluster analysis, density projection calculations, and diffusion coefficient calculation of water molecules within the resin matrix. MD simulations results are further used to understand the interaction of water molecules with the resin matrix comprehensively, which governs the composite's mechanical properties. The water sorption study showed that the MAPOSS composite has less water sorption capacity than the MIPOSS composite. The practical significance of this study is to find properties that affect dental restoration and longevity, which can help in the design of better materials for dental applications.

Structure and dynamics of confined water: Selected examples

The purpose of this paper is to account for selected examples about the structure and the dynamics of confined water as a function of temperature. Examples for the interactions of water molecules with model systems developing either hydrophilic/ hydrophobic interactions or both, as well as with biological macromolecules are presented. The static and transport properties of confined water are compared with that of bulk water.