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The objective of this work was to improve the solubility and discover a stable co-amorphous form of valsartan (VAL), a BCS class-II drug, by utilizing small molecule 2-Aminopyridine (2-AP) in varying molar ratios (2:1, 1:1, and 1:2), employing a solvent evaporation technique. Additionally, by way of a density functional theory (DFT)-based computational method with commercially available software, a new approach for determining the intermolecular connectivity of multi-molecular hydrogen bonding systems was proposed. The binary systems’ features were characterized by PXRD, DSC, FTIR, and Raman spectroscopy, while the equilibrium solubility and dissolution was determined in 0.1 N HCL and water conditions to investigate the dissolution advantage of the prepared co-amorphous systems. The results demonstrated that the co-amorphous system was successfully prepared in VAL/2-AP with a 1:2 molar ratio following solvent evaporation, whereby the hydrogen bonding sites of VAL were fully occupied. Physical stability studies were carried out under dry conditions at room temperature for 6 months. Furthermore, four possible ternary systems were constructed, and their vibrational modes were simulated by DFT calculations. The calculated infrared spectra of the four configurations varied widely, with trimer 1 showing the most resemblance to the experimental spectrum of the co-amorphous 1:2 system. Additionally, co-amorphous VAL/2-AP displayed significant improvement in the solubility and dissolution study. Notably, in the 1:2 ratio, there was almost a 4.5-fold and 15.6-fold increase in VAL’s solubility in 0.1 N HCL and water environments, respectively. In conclusion, our findings highlight the potential of co-amorphous systems as a feasible approach to improving the properties and bioavailabilities of insoluble drugs. The proposed simulation method provides valuable insights into determining the supramolecular structure of multi-molecular hydrogen bonding systems, offering a novel perspective for investigating such systems.

The combination of Al nanoparticles (ANPs) as fuel and H2O2 as oxidizer is a potential green space propellant. In this research, reactive force field molecular dynamics (ReaxFF-MD) simulations were used to study the influence of water addition on the combustion of Al/H2O2. The MD results showed that as the percentage of H2O increased from 0 to 30%, the number of Al-O bonds on the ANPs decreased, the number of Al-H bonds increased, and the adiabatic flame temperature of the system decreased from 4612 K to 4380 K. Since the Al-O bond is more stable, as the simulation proceeds, the number of Al-O bonds will be significantly higher than that of Al-H and Al-OH bonds, and the Al oxides (Al[O]x) will be transformed from low to high coordination. Subsequently, the combustion mechanism of the Al/H2O2/H2O system was elaborated from an atomic perspective. Both H2O2 and H2O were adsorbed and chemically activated on the surface of ANPs, resulting in molecular decomposition into free radicals, which were then captured by ANPs. H2 molecules could be released from the ANPs, while O2 could not be released through this pathway. Finally, it was found that the coverage of the oxide layer reduced the rate of H2O2 consumption and H2 production significantly, simultaneously preventing the deformation of the Al clusters’ morphology.

The relationship between structure and reactivity plays a dominant role in water dissociation on the various TiO2 crystallines. To observe the adsorption and dissociation behavior of H2O, the reaction force field (ReaxFF) is used to investigate the dynamic behavior of H2O on rutile (110) and anatase (101) surfaces in an aqueous environment. Simulation results show that there is a direct proton transfer between the adsorbed H2O (H2Oad) and the bridging oxygen (Obr) on the rutile (110) surface. Compared with that on the rutile (110) surface, an indirect proton transfer occurs on the anatase (101) surface along the H-bond network from the second layer of water. This different mechanism of water dissociation is determined by the distance between the 5-fold coordinated Ti (Ti5c) and Obr of the rutile and anatase TiO2 surfaces, resulting in the direct or indirect proton transfer. Additionally, the hydrogen bond (H-bond) network plays a crucial role in the adsorption and dissociation of H2O on the TiO2 surface. To describe interfacial water structures between TiO2 and bulk water, the double-layer model is proposed. The first layer is the dissociated H2O on the rutile (110) and anatase (101) surfaces. The second layer forms an ordered water structure adsorbed to the surface Obr or terminal OH group through strong hydrogen bonding (H-bonding). Affected by the H-bond network, the H2O dissociation on the rutile (110) surface is inhibited but that on the anatase (101) surface is promoted.

By means of a computational method based on Density Functional Theory (DFT), using commercially available software, a novel method for simulating equilibrium geometry harmonic vibrational frequencies is proposed. Finasteride, Lamivudine, and Repaglinide were selected as model molecules to study the adaptability of the new method. Three molecular models, namely the single-molecular, central-molecular, and multi-molecular fragment models, were constructed and calculated by Generalized Gradient Approximations (GGAs) with the PBE functional via the Material Studio 8.0 program. Theoretical vibrational frequencies were assigned and compared to the corresponding experimental data. The results indicated that the traditional single-molecular calculation and scaled spectra with scale factor exhibited the worst similarity for all three pharmaceutical molecules among the three models. Furthermore, the central-molecular model with a configuration closer to the empirical structure resulted in a reduction of mean absolute error (MAE) and root mean squared error (RMSE) in all three pharmaceutics, including the hydrogen-bonded functional groups. However, the improvement in computational accuracy for different drug molecules using the central-molecular model for vibrational frequency calculation was unstable. Whereas, the new multi-molecular fragment interception method showed the best agreement with experimental results, exhibiting MAE and RMSE values of 8.21 cm−1 and 18.35 cm−1 for Finasteride, 15.95 cm−1 and 26.46 cm−1 for Lamivudine, and 12.10 cm−1 and 25.82 cm−1 for Repaglinide. Additionally, this work provides comprehensive vibrational frequency calculations and assignments for Finasteride, Lamivudine, and Repaglinide, which have never been thoroughly investigated in previous research.

Previous studies have been carried out on the effect of silica nanoparticles (SNPs) on the stability of oil–water emulsions. However, the combining configuration of SNPs and oil droplets at the molecular level and the effect of SNP content on the coalescence behavior of oil droplets cannot be obtained through experiments. In this paper, molecular dynamics (MD) simulation was performed to investigate the adsorption configuration of hydrophilic SNPs in an O/W emulsion system, and the effect of adsorption of SNPs on coalescence of oil droplets. The simulation results showed: (i) SNPs adsorbed on the surface of oil droplets, and excessive SNPs self-aggregated and connected by hydrogen bonds. (ii) Partially hydrophilic asphaltene and resin molecules formed adsorption configurations with SNPs, which changed the distribution of oil droplet components. Furthermore, compared with hydrophobic asphaltene, the hydrophilic asphaltene was easier to combine with SNPs. (iii) SNPs would extend the oil droplet coalescence time, and the π–π stacking structures were formed between asphaltene and asphaltene or resin molecules to enhance the connection between oil droplets during the oil droplet contact process. (iv) Enough SNPs tightly wrapped around the oil droplet, similar to the formation of a rigid film on the surface of an oil droplet, which hindered the contact and coalescence of components between oil droplets.

Summary: It is of great importance and practical value to develop a facile and operable surface treatment method of materials with excellent antipollution and antiadhesion property, but still a huge challenge. In this work, a series of pseudo-zwitterions are prepared from electrostatic assembly of cationic polyethyleneimine and anionic phosphonic clusters. These pseudo-zwitterionic assemblies provide a strong hydration through electrostatic interaction with water and in turn create a barrier against oil foulants, leading to a nearly zero crude oil adhesion force. The pseudo-zwitterions-decorated surfaces exhibit exceptional water-cleanable oil-repellent property, even when they are completely dried and without prehydration before fouled by crude oil. While using these pseudo-zwitterions-modified polymeric membranes for separating surfactant stabilized oil-in-water emulsion, less than 10% decline of permeating flux is observed throughout a 2-h continuous separation experiment, showing excellent emulsion separation ability and antipollution performance for high viscous oil.

Zwitterionic polymers as crucial antifouling materials exhibit excellent antifouling performance due to their strong hydration ability. The structure–property relationship at the molecular level still remains to be elucidated. In this work, the surface hydration ability of three antifouling polymer membranes grafting on polysiloxane membranes Poly(sulfobetaine methacrylate) (T4-SB), poly(3-(methacryloyloxy)propane-1-sulfonate) (T4-SP), and poly(2-(dimethylamino)ethyl methacrylate) (T4-DM) was investigated. An orderly packed, and tightly bound surface hydration layer above T4-SP and T4-SB antifouling membranes was found by means of analyzing the dipole orientation distribution, diffusion coefficient, and average residence time. To further understand the surface hydration ability of three antifouling membranes, the surface structure, density profile, roughness, and area percentage of hydrophilic surface combining electrostatic potential, RDFs, SDFs, and noncovalent interactions of three polymers’ monomers were studied. It was concluded that the broadest distribution of electrostatic potential on the surface and the nature of anionic SO3- groups led to the following antifouling order of T4-SB > T4-SP > T4-DM. We hope that this work will gain some insight for the rational design and optimization of ecofriendly antifouling materials.

A bidirectional pulsed electric field (BPEF) method is considered a simple and novel technique to demulsify O/W emulsions. In this paper, molecular dynamics simulation was used to investigate the transformation and aggregation behavior of oil droplets in O/W emulsion under BPEF. Then, the effect of surfactant (sodium dodecyl sulfate, SDS) on the demulsification of O/W emulsion was investigated. The simulation results showed that the oil droplets transformed and moved along the direction of the electric field. SDS molecules can shorten the aggregation time of oil droplets in O/W emulsion. The electrostatic potential distribution on the surface of the oil droplet, the elongation length of the oil droplets, and the mean square displacement (MSD) of SDS and asphaltene molecules under an electric field were calculated to explain the aggregation of oil droplets under the simulated pulsed electric field. The simulation also showed that the two oil droplets with opposite charges have no obvious effect on the aggregation of the oil droplets. However, van der Waals interactions between oil droplets was the main factor in the aggregation.

CO2 enhanced oil recovery (CO2-EOR) has become significantly crucial to the petroleum industry, in particular, CO2 miscible flooding can greatly improve the efficiency of EOR. Minimum miscibility pressure (MMP) is a vital factor affecting CO2 flooding, which determines the yield and economic benefit of oil recovery. Therefore, it is important to predict this property for a successful field development plan. In this study, a novel model based on molecular dynamics to determine MMP was developed. The model characterized a miscible state by calculating the ratio of CO2 and crude oil atoms that pass through the initial interface. The whole process was not affected by other external objective factors. We compared our model with several famous empirical correlations, and obtained satisfactory results—the relative errors were 8.53% and 13.71% for the two equations derived from our model. Furthermore, we found the MMPs predicted by different reference materials (i.e., CO2/crude oil) were approximately linear (R2 = 0.955). We also confirmed the linear relationship between MMP and reservoir temperature (TR). The correlation coefficient was about 0.15 MPa/K in the present study.

Heavy oil in crude oil flooding is extremely difficult to extract due to its high viscosity and poor fluidity. In this paper, molecular dynamics simulation was used to study the emulsification behavior of sodium dodecyl sulfonate (SDSn) micelles on heavy oil droplets composed of asphaltenes (ASP) at the molecular level. Some analyzed techniques were used including root mean square displacement, hydrophile-hydrophobic area of an oil droplet, potential of mean force, and the number of hydrogen bonds between oil droplet and water phase. The simulated results showed that the asphaltene with carboxylate groups significantly enhances the hydration layer on the surface of oil droplets, and SDSn molecules can change the strength of the hydration layer around the surface of the oil droplets. The water bridge structure between both polar heads of the surfactant was commonly formed around the hydration layer of the emulsified oil droplet. During the emulsification of heavy oil, the ratio of hydrophilic hydrophobic surface area around an oil droplet is essential. Molecular dynamics method can be considered as a helpful tool for experimental techniques at the molecular level.

Using salicylic acid and acetic anhydride as raw materials, silica gel as a catalyst, and microwave technology as an optimization method, the university organic chemistry teaching experiment of 'Preparation and Characterization of Acetylsalicylic Acid' was improved. Through the experiment, the impact of factors such as microwave power, reaction time, and raw material ratio on the final yield was explored. The optimal experimental conditions were determined as follows: silica gel with a particle size of 100-200 mesh, 0.25 g in quantity, 60 s reaction time, 70 °C reaction temperature, 500 W microwave power, and a molar ratio of acetic anhydride to salicylic acid of 2 : 1. The average yield was approximately 68.0%. Compared to the conventional heating method for the preparation of acetylsalicylic acid, microwave-assisted synthesis offers advantages such as simplicity, shorter reaction time, higher product yield, fewer impurities, and environmental friendliness. Introducing this microwave experiment into undergraduate organic chemistry laboratory teaching can broaden students' horizons, enrich experimental teaching content, and further improve the teaching level. [ABSTRACT FROM AUTHOR]

This experiment introduces the application of chemistry in archaeology through the detection and analysis of alcoholic beverage residues in pottery. Organic acids which are the indicators of alcoholic beverage residues are extracted through a series of experimental steps such as extraction, filtration, centrifugation and rotary evaporation, and measured by High Performance Liquid Chromatography (HPLC). Combined with archaeological background of pottery, the results of this experiment can be used to analyze the possible usage of the pottery. Based on emerging interdisciplinary archaeological chemistry, this experiment is offered to students majoring in chemistry and archaeology, which could provide insights into fundamental concepts, basic methods of sample isolation and HPLC analysis, as well as provide primary perception of the focused topic in archaeology. [ABSTRACT FROM AUTHOR]