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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Physical Chemistry".

Deadline for manuscript submissions: closed (30 April 2021) | Viewed by 24590

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Prof. Dr. Carlos Bravo Díaz

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Department of Physical Chemistry, Faculty of Chemistry, Universidade de Vigo, 36200 Vigo, Spain
Interests: lipid oxidation; antioxidants; antioxidant distribution; antioxidant efficiency; emulsion; polyunsaturated fatty acids; oxidative stress; reactive oxygen species; modelling reaction kinetics; emulsifiers
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Dr. Sonia Losada-Barreiro

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Dear Colleagues,

This Special Issue on interfacial chemistry aims to provide researchers with a state-of-the-art of the different phenomena that take place at phase boundaries or interfaces, bringing readers the latest developments in the field. Interfacial chemistry is a field with unlimited potential, as the chemical and physical properties and processes at the interfaces are the scientific basis for so many of the technologies that affect our lives, creating new opportunities. The chemistry of the living systems is largely controlled by biomembranes, but their complexity ensures that increasing efforts are devoted to creating and characterizing artificial model systems such as micelles, reverse micelles, micro- and macro-emulsions, liposomes, and so on.

Interfaces play a key role in a number of diverse phenomena, including catalysis, biosensing, electrochemical processes, as well as many others. Systems with interfaces are present in an infinite number of different industrial processes and physicochemical phenomenon, and have an unlimited number of uses that involves every industry and every aspect of life, from pharmaceuticals, medicine, food processing, cleaning, paints, and so on. Their applications depend on the applied properties and the mechanisms of action, and therefore, the design of the functionalized materials and their optimization relies on an intimate understanding of “structure–activity” relationships.

Research manuscripts and reviews are welcome. Our aim is to improve the general understanding of the role of interfaces in chemical reactivity. The interfacial region is of a few nanometers thick and has different solvent properties than those of the bulk liquids. Its tendency to concentrate or separate reactants, together with its ability to orientate molecules, makes them excellent systems to analyze a variety of phenomena. Interfaces cannot be isolated without disrupting the existing equilibria, and the exchange of reactants between the interface and the adjacent bulk solution(s) may be superimposed to the interfacial reaction. Molecules of the reactant arrive at an interface from the bulk solution by random motion (diffusion), and the reactant molecules must remain at the interface for some time. The rate of chemical reactions taking place at an interface depend, first, on how fast the reactants reach the interface, and, in some instances, on the removal of products, leaving the interface vacant for further reactions. Moreover, because of the spatially heterogeneous and dynamic nature of interfacial reactions, there is a recognized need for localized measurements and characterizations under the relevant reaction conditions.

Dr. Carlos Bravo-Diaz
Dr. Sonia Losada-Barreiro
Guest Editors

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Keywords

Surfactant (natural and synthetic)-based systems
Association colloids, emulsions, and nano-emulsions
Modelization of chemical reactivity in multiphasic systems
Physical organic chemistry
Bioderived and bioinspired surfactants
Food emulsions

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Published Papers (7 papers)

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Research

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16 pages, 1416 KiB

Open AccessArticle

Methyl-Cyclohexane Methanol (MCHM) Isomer-Dependent Binding on Amorphous Carbon Surfaces

by William A. Alexander

Molecules 2021, 26(11), 3411; https://doi.org/10.3390/molecules26113411 - 4 Jun 2021

Cited by 1 | Viewed by 3243

Abstract

In January 2014, over 10,000 gallons of methyl-cyclohexane methanol (MCHM) leaked into the Elk River in West Virginia, in a chemical spill incident that contaminated a large portion of the state’s water supply and left over 300,000 residents without clean water for many days and weeks. Initial efforts to remove MCHM at the treatment plant centered on the use of granulated activated carbon (GAC), which removed some of the chemical from the water, but MCHM levels were not lowered to a “non-detect” status until well after the chemical plume had moved downstream of the intake. Months later, MCHM was again detected at the outflow (but not the inflow) at the water treatment facility, necessitating the full and costly replacement of all GAC in the facility. The purpose of this study is to investigate the hypothesis that preferential absorbance of one of the two MCHM isomers, coupled with seasonal variations in water temperature, explain this contrary observation. Calculated intermolecular potentials between ovalene (a large planar polycyclic aromatic hydrocarbon) and the MCHM isomers were compared to physisorption potentials of MCHM onto an amorphous carbon model. While a molecular mechanics (MM) force field predicts no difference in the average interaction potentials between the cis- and trans-MCHM with the planar ovalene structure, MM predicts that the trans isomer binds stronger than the cis isomer to the amorphous carbon surface. Semi-empirical and density functional theory also predict stronger binding of trans-MCHM on both the planar and amorphous surfaces. The differences in the isomer binding strengths on amorphous carbon imply preferential absorbance of the trans isomer onto activated charcoal filter media. Considering seasonal water temperatures, simple Arrhenius kinetics arguments based on these predicted binding energies help explain the environmental observations of MCHM leeching from the GAC filters months after the spill. Overall, this work shows the important implications that can arise from detailed interfacial chemistry investigations. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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11 pages, 1778 KiB

Open AccessCommunication

The Isoelectric Point of an Exotic Oxide: Tellurium (IV) Oxide

by Marek Kosmulski and Edward Mączka

Molecules 2021, 26(11), 3136; https://doi.org/10.3390/molecules26113136 - 24 May 2021

Cited by 6 | Viewed by 2239

Abstract

The pH-dependent surface charging of tellurium (IV) oxide has been studied. The isoelectric point (IEP) of tellurium (IV) oxide was determined by microelectrophoresis in various 1-1 electrolytes over a concentration range of 0.001–0.1 M. In all electrolytes studied and irrespective of their concentration the zeta potential of TeO₂ was negative over the pH range 3–12. In other words the IEP of TeO₂ is at pH below 3 (if any). TeO₂ specifically adsorbs ionic surfactants, and their presence strongly affects the zeta potential. In contrast the effect of multivalent inorganic ions on the zeta potential of TeO₂ is rather insignificant (no shift in the IEP). In this respect TeO₂ is very different from metal oxides. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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12 pages, 3734 KiB

Open AccessArticle

Facile Electrochemical Method for the Fabrication of Stable Corrosion-Resistant Superhydrophobic Surfaces on Zr-Based Bulk Metallic Glasses

by Mengmeng Yu, Ming Zhang, Jing Sun, Feng Liu, Yujia Wang, Guanzhong Ding, Xiubo Xie, Li Liu, Xiangjin Zhao and Haihong Li

Molecules 2021, 26(6), 1558; https://doi.org/10.3390/molecules26061558 - 12 Mar 2021

Cited by 8 | Viewed by 2020

Abstract

Both surface microstructure and low surface energy modification play a vital role in the preparation of superhydrophobic surfaces. In this study, a safe and simple electrochemical method was developed to fabricate superhydrophobic surfaces of Zr-based metallic glasses with high corrosion resistance. First, micro–nano composite structures were generated on the surface of Zr-based metallic glasses by electrochemical etching in NaCl solution. Next, stearic acid was used to decrease surface energy. The effects of electrochemical etching time on surface morphology and wettability were also investigated through scanning electron microscopy and contact angle measurements. Furthermore, the influence of micro–nano composite structures and roughness on the wettability of Zr-based metallic glasses was analysed on the basis of the Cassie–Baxter model. The water contact angle of the surface was 154.3° ± 2.2°, and the sliding angle was <5°, indicating good superhydrophobicity. Moreover, the potentiodynamic polarisation test and electrochemical impedance spectroscopy suggested excellent corrosion resistance performance, and the inhibition efficiency of the superhydrophobic surface reached 99.6%. Finally, the prepared superhydrophobic surface revealed excellent temperature-resistant and self-cleaning properties. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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14 pages, 1776 KiB

Open AccessArticle

Reflection Absorption Infrared Spectroscopy Characterization of SAM Formation from 8-Mercapto-N-(phenethyl)octanamide Thiols with Phe Ring and Amide Groups

by Zenonas Kuodis, Ieva Matulaitienė, Marija Špandyreva, Linas Labanauskas, Sigitas Stončius, Olegas Eicher-Lorka, Rita Sadzevičienė and Gediminas Niaura

Molecules 2020, 25(23), 5633; https://doi.org/10.3390/molecules25235633 - 30 Nov 2020

Cited by 11 | Viewed by 4269

Abstract

Multifunctional amide-containing self-assembled monolayers (SAMs) provide prospects for the construction of interfaces with required physicochemical properties and distinctive stability. In this study, we report the synthesis of amide-containing thiols with terminal phenylalanine (Phe) ring functionality (HS(CH₂)₇CONH(CH₂)₂C₆H₅) and the characterization of the formation of SAMs from these thiols on gold by reflection absorption infrared spectroscopy (RAIRS). For reliable assignments of vibrational bands, ring deuterated analogs were synthesized and studied as well. Adsorption time induced changes in Amide-II band frequency and relative intensity of Amide-II/Amide-I bands revealed two-state sigmoidal form dependence with a transition inflection points at 2.2 ± 0.5 and 4.7 ± 0.5 min, respectively. The transition from initial (disordered) to final (hydrogen-bonded, ordered) structure resulted in increased Amide-II frequency from 1548 to 1557 cm⁻¹, which is diagnostic for a strongly hydrogen-bonded amide network in trans conformation. However, the lateral interactions between the alkyl chains were found to be somewhat reduced when compared with well-ordered alkane thiol monolayers. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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16 pages, 4087 KiB

Open AccessArticle

Preparation and Characterization of Octenyl Succinate β-Cyclodextrin and Vitamin E Inclusion Complex and Its Application in Emulsion

by Dongmei Ke, Wenxue Chen, Weijun Chen, Yong-Huan Yun, Qiuping Zhong, Xiaotang Su and Haiming Chen

Molecules 2020, 25(3), 654; https://doi.org/10.3390/molecules25030654 - 4 Feb 2020

Cited by 16 | Viewed by 3859

Abstract

Vitamin E (VE) and β-cyclodextrin (β-CD) can form an inclusion complex; however, the inclusion rate is low because of the weak interaction between VE and β-CD. The results of a molecular docking study showed that the oxygen atom in the five-membered ring of octenyl succinic anhydride (OSA) formed a strong hydrogen bond interaction (1.89 Å) with the hydrogen atom in the hydroxyl group of C-6. Therefore, β-CD was modified using OSA to produce octenyl succinic-β-cyclodextrin (OCD). The inclusion complexes were then prepared using OCD with VE. The properties of the inclusion complex were investigated by Fourier-transform infrared spectroscopy (FT-IR), ¹³C CP/MAS NMR, scanning electron microscopy (SEM), and atomic force microscopy (AFM). The results demonstrated that VE had been embedded into the cavity of OCD. Furthermore, the emulsifying properties (particle size distribution, ζ-potential, and creaming index) of the OCD/VE inclusion-complex-stabilized emulsion were compared with that stabilized by β-CD, OCD, and an OCD/VE physical mixture. The results showed that the introduction of the OS group and VE could improve the physical stability of the emulsion. In addition, the OCD/VE inclusion complex showed the strongest ability to protect the oil in the emulsion from oxidation. OCD/VE inclusion complex was able to improve the physical and oxidative stability of the emulsion, which is of great significance to the food industry. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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12 pages, 2643 KiB

Open AccessArticle

Effects of Molecular Weight and Guluronic Acid/Mannuronic Acid Ratio on the Rheological Behavior and Stabilizing Property of Sodium Alginate

by Wenxiao Jiao, Wenxue Chen, Yuqi Mei, Yonghuan Yun, Boqiang Wang, Qiuping Zhong, Haiming Chen and Weijun Chen

Molecules 2019, 24(23), 4374; https://doi.org/10.3390/molecules24234374 - 29 Nov 2019

Cited by 66 | Viewed by 5032

Abstract

The aim of this study was to prepare sodium alginates (SAs) with different molecular weight and G/M ratio, and characterize their rheological behaviors and emulsifying properties. The result of Fourier transform infrared (FTIR) showed that the chemical bonds among the β-d-mannuronic acid- (M-), α-l-guluronic acid- (G-), and MG-sequential blocks in the SA chains were not changed significantly by acid treatment. Meanwhile, the molecular weight and G/M ratio of the SA exhibited drastic variation after acid modification. The result of rheological analysis suggesting that the apparent viscosity of SA reduced from 30 to 16.4 mPa.s with the increase of shear rate, reveals that SA solution belongs to pseudoplastic liquid. Also, the apparent viscosity of acid-modified SA solution dropped rapidly with the decrease of the molecular weight. The properties of emulsions stabilized by SA, SA-Ms, and commercial SAs were evaluated via the interface tensiometry and determination of the zeta potential, droplet size, creaming index (CI), and Turbiscan stability index (TSI). Compared with the SA-stabilized emulsion, the interfacial tension of the emulsion stabilized by SA-M increased with the decrease of the molecular weight reduced at the similar M/G ratio. The decrease in zeta potential and the increase in TSI of the emulsion were observed with the decrease of molecular weight, indicating that molecular weight plays an important role on the emulsifying ability of SA. In addition, the SA with low G/M ratio can form emulsions with stable and fine droplets. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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Review

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25 pages, 5692 KiB

Open AccessReview

Modeling Chemical Reactivity at the Interfaces of Emulsions: Effects of Partitioning and Temperature

by Marlene Costa, Fátima Paiva-Martins, Sonia Losada-Barreiro and Carlos Bravo-Díaz

Molecules 2021, 26(15), 4703; https://doi.org/10.3390/molecules26154703 - 3 Aug 2021

Cited by 14 | Viewed by 2939

Abstract

Bulk phase chemistry is hardly ever a reasonable approximation to interpret chemical reactivity in compartmentalized systems, because multiphasic systems may alter the course of chemical reactions by modifying the local concentrations and orientations of reactants and by modifying their physical properties (acid-base equilibria, redox potentials, etc.), making them—or inducing them—to react in a selective manner. Exploiting multiphasic systems as beneficial reaction media requires an understanding of their effects on chemical reactivity. Chemical reactions in multiphasic systems follow the same laws as in bulk solution, and the measured or observed rate constant of bimolecular reactions can be expressed, under dynamic equilibrium conditions, in terms of the product of the rate constant and of the concentrations of reactants. In emulsions, reactants distribute between the oil, water, and interfacial regions according to their polarity. However, determining the distributions of reactive components in intact emulsions is arduous because it is physically impossible to separate the interfacial region from the oil and aqueous ones without disrupting the existing equilibria and, therefore, need to be determined in the intact emulsions. The challenge is, thus, to develop models to correctly interpret chemical reactivity. Here, we will review the application of the pseudophase kinetic model to emulsions, which allows us to model chemical reactivity under a variety of experimental conditions and, by carrying out an appropriate kinetic analysis, will provide important kineticparameters. Full article

(This article belongs to the Special Issue Interfacial Chemistry)

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