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Amphiphilic Molecules, Interfaces and Colloids

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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: 31 October 2024 | Viewed by 3789

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Dr. Khristo Khristov

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Guest Editor

Institute of Physical Chemistry, Bulgarian Academy of Science, 1113 Sofia, Bulgaria
Interests: emulsions and foams; thin liquid films; interfacial and bulk rheology; heavy crude oil; petroleum emulsions; electrochemical impedance spectroscopy of thin film; self-assembly

Dr. Plamen Tchoukov

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Guest Editor

Institute of Physical Chemistry, Bulgarian Academy of Sciences, 1113 Sofia, Bulgaria
Interests: emulsions and foams; thin liquid films; interfacial and bulk rheology; heavy crude oil; petroleum emulsions; electrochemical impedance spectroscopy of thin film; self-assembly
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Special Issue Information

Dear Colleagues,

Colloids, such as emulsions, foams, sols, and gels, play an integral role in living organisms, the natural environment, resource extraction, pharmaceuticals, cleaning products, processing industries, and in almost all aspects of our everyday life. To a large extent, colloid stability and functionality are defined by the properties of interfaces between dispersed and continuous phases and by the surface forces acting at the micro- and nanoscale levels. It is the amphiphilic molecules that are capable of altering colloidal system properties, thus changing the overall system behavior. This is why a comprehensive understanding of amphiphile molecular structure and the respective interactions taking place at the interfaces ensures an effective control over colloidal system properties.

For this Special Issue, we welcome contributions which highlight the relation between amphiphile molecular structure, self-assembly in solutions, molecular arrangements at interfaces, specific interactions at micro- and nanoscale, and the properties displayed by the colloidal systems. Suitable research will span from fundamental studies on the physicochemical behavior of colloidal systems to the design of innovative solutions for practical applications.

Dr. Khristo Khristov
Dr. Plamen Tchoukov
Guest Editors

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Keywords

emulsions
foams
sols
gels
amphiphilic molecules
self-assembled structures
phase behavior
surface forces
intermolecular forces
adsorption
rheology
design of functionalized colloids
thin liquid films

Published Papers (7 papers)

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Research

15 pages, 2733 KiB

Open AccessArticle

Capillarity in Interfacial Liquids and Marbles: Mechanisms, Properties, and Applications

by Yang Liu, Yuanfeng Wang and John H. Xin

Molecules 2024, 29(13), 2986; https://doi.org/10.3390/molecules29132986 - 23 Jun 2024

Viewed by 363

Abstract

The mechanics of capillary force in biological systems have critical roles in the formation of the intra- and inter-cellular structures, which may mediate the organization, morphogenesis, and homeostasis of biomolecular condensates. Current techniques may not allow direct and precise measurements of the capillary forces at the intra- and inter-cellular scales. By preserving liquid droplets at the liquid–liquid interface, we have discovered and studied ideal models, i.e., interfacial liquids and marbles, for understanding general capillary mechanics that existed in liquid-in-liquid systems, e.g., biomolecular condensates. The unexpectedly long coalescence time of the interfacial liquids revealed that the Stokes equation does not hold as the radius of the liquid bridge approaches zero, evidencing the existence of a third inertially limited viscous regime. Moreover, liquid transport from a liquid droplet to a liquid reservoir can be prohibited by coating the droplet surface with hydrophobic or amphiphilic particles, forming interfacial liquid marbles. Unique characteristics, including high stability, transparency, gas permeability, and self-assembly, are observed for the interfacial liquid marbles. Phase transition and separation induced by the formation of nanostructured materials can be directly observed within the interfacial liquid marbles without the need for surfactants and agitation, making them useful tools to research the interfacial mechanics. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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19 pages, 2534 KiB

Open AccessArticle

Aggregation Behavior and Application Properties of Novel Glycosylamide Quaternary Ammonium Salts in Aqueous Solution

by Yunkai Wang, Zeyu Chen, Erzhuang Zhang, Lifei Zhi, Martino Di Serio, Guoyong Wang, Yan Wang, Xiaoming Li, Xudong Liu and Ying Huang

Molecules 2024, 29(12), 2749; https://doi.org/10.3390/molecules29122749 - 9 Jun 2024

Viewed by 469

Abstract

Amidation of lactobionic acid with N,N-dimethylaminopropyltriamine was conducted to obtain N-(3′-dimethylaminopropyl)-lactamido-3-aminopropane (DDLPD), which was quaternized with bromoalkanes of different carbon chain lengths to synthesize double-stranded lactosylamide quaternary ammonium salt N-[N′[3-(lactosylamide)]propyl-N′-alkyl] propyl-N,N-dimethyl-N-alkylammonium bromide (C_nDDLPB, n = 8, 10, 12, 14, 16). The surface activity and the adsorption and aggregation behaviors of the surfactants were investigated via equilibrium surface tension, dynamic light scattering, and cryo-electron microscopy measurements in an aqueous solution. The application properties of the products in terms of wettability, emulsification, foam properties, antistatic, salt resistance, and bacteriostatic properties were tested. C_nDDLPB exhibited a low equilibrium surface tension of 27.82 mN/m. With an increase in the carbon chain length, the critical micellar concentration of C_nDDLPBD decreased. Cryo-electron microscopy revealed that all products except C₈DDLPB formed stable monolayer, multi-layer, and multi-compartmental vesicle structures in an aqueous solution. C₁₄DDLPB has the best emulsification performance on soybean oil, with a time of 16.6 min; C₁₄DDLPB has good wetting and spreading properties on polytetrafluoroethylene (PTFE) when the length of carbon chain is from 8 to 14, and the contact angle can be lowered to 33°~40°; C_nDDLPB has low foam, which is typical of low-foaming products; C₈DDLPB and C₁₀DDLPB both show good antistatic properties. C₈DDLPB and C₁₄DDLPB have good salt resistance, and C₁₂DDLPB has the best antimicrobial property, with the inhibition rate of 99.29% and 95.28% for E. coli and Gluconococcus aureus, respectively, at a concentration of 350 ppm. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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14 pages, 2568 KiB

Open AccessArticle

Dispersive Solid Phase Extraction of Melatonin with Graphene/Clay Mixtures and Fluorescence Analysis in Surfactant Aqueous Solutions

by Lucía Gutiérrez-Fernández, Ana M. Díez-Pascual and María Paz San Andrés

Molecules 2024, 29(11), 2699; https://doi.org/10.3390/molecules29112699 - 6 Jun 2024

Viewed by 338

Abstract

In this work, the dispersive solid phase extraction (dSPE) of melatonin using graphene (G) mixtures with sepiolite (SEP) and bentonite (BEN) clays as sorbents combined with fluorescence detection has been investigated. The retention was found to be quantitative for both G/SEP and G/BEN 4/96 and 10/90 w/w mixtures. G/clay 4/96 w/w mixtures were selected to study the desorption process since the retention was weaker, thus leading to easier desorption. MeOH and aqueous solutions of the nonionic surfactant Brij L23 were tested as desorbents. For both clays and an initial sample volume of 25 mL, a percentage of melatonin recovery close to 100% was obtained using 10 or 25 mL of MeOH as desorbent. Further, using a G/SEP mixture, 25 mL as the initial sample volume and 5 mL of MeOH or 60 mM Brij L23 solution as the desorbent, recoveries of 98.3% and 90% were attained, respectively. The whole method was applied to herbal tea samples containing melatonin, and the percentage of agreement with the labeled value was 86.5%. It was also applied to herbal samples without melatonin by spiking them with two concentrations of this compound, leading to recoveries of 100 and 102%. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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15 pages, 6633 KiB

Open AccessArticle

A Fusion–Growth Protocell Model Based on Vesicle Interactions with Pyrite Particles

by Dong Guo, Ziyue Zhang, Jichao Sun, Hui Zhao, Wanguo Hou and Na Du

Molecules 2024, 29(11), 2664; https://doi.org/10.3390/molecules29112664 - 4 Jun 2024

Viewed by 358

Abstract

Protocell models play a pivotal role in the exploration of the origin of life. Vesicles are one type of protocell model that have attracted much attention. Simple single-chain amphiphiles (SACs) and organic small molecules (OSMs) possess primitive relevance and were most likely the building blocks of protocells on the early Earth. OSM@SAC vesicles have been considered to be plausible protocell models. Pyrite (FeS₂), a mineral with primitive relevance, is ubiquitous in nature and plays a crucial role in the exploration of the origin of life in the mineral–water interface scenario. “How do protocell models based on OSM@SAC vesicles interact with a mineral–water interface scenario that simulates a primitive Earth environment” remains an unresolved question. Hence, we select primitive relevant sodium monododecyl phosphate (SDP), isopentenol (IPN) and pyrite (FeS₂) mineral particles to build a protocell model. The model investigates the basic physical and chemical properties of FeS₂ particles and reveals the effects of the size, content and duration of interaction of FeS₂ particles on IPN@SDP vesicles. This deepens the understanding of protocell growth mechanisms in scenarios of mineral–water interfaces in primitive Earth environments and provides new information for the exploration of the origin of life. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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20 pages, 2457 KiB

Open AccessArticle

Sugar-Based Surfactants: Effects of Structural Features on the Physicochemical Properties of Sugar Esters and Their Comparison to Commercial Octyl Glycosides

by Huiling Lu, Gwladys Pourceau, Benoit Briou, Anne Wadouachi, Théophile Gaudin, Isabelle Pezron and Audrey Drelich

Molecules 2024, 29(10), 2338; https://doi.org/10.3390/molecules29102338 - 16 May 2024

Viewed by 445

Abstract

Two series of sugar esters with alkyl chain lengths varying from 5 to 12 carbon atoms, and with a head group consisting of glucose or galactose moieties, were synthesized. Equilibrium surface tension isotherms were measured, yielding critical micellar concentration (CMC) surface tensions at CMC (γcmc) and minimum areas at the air–water interface (Amin). In addition, Krafft temperatures (Tks) were measured to characterize the ability of molecules to dissolve in water, which is essential in numerous applications. As a comparison to widely used commercial sugar-based surfactants, those measurements were also carried out for four octyl d-glycosides. Impacts of the linkages between polar and lipophilic moieties, alkyl chain lengths, and the nature of the sugar head group on the measured properties were highlighted. Higher Tk and, thus, lower dissolution ability, were found for methyl 6-O-acyl-d-glucopyranosides. CMC and γcmc decreased with the alkyl chain lengths in both cases, but Amin did not appear to be influenced. Both γcmc and Amin appeared independent of the ester group orientation. Notably, alkyl (methyl α-d-glucopyranosid)uronates were found to result in noticeably lower CMC, possibly due to a closer distance between the carbonyl function and the head group. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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16 pages, 5059 KiB

Open AccessArticle

Co-Assembled Supramolecular Organohydrogels of Amphiphilic Zwitterion and Polyoxometalate with Controlled Microstructures

by Peilin Wei, Yu Duan, Chen Wang, Panpan Sun and Na Sun

Molecules 2024, 29(10), 2286; https://doi.org/10.3390/molecules29102286 - 12 May 2024

Viewed by 724

Abstract

The organization of modifiable and functional building components into various superstructures is of great interest due to their broad applications. Supramolecular self-assembly, based on rationally designed building blocks and appropriately utilized driving forces, is a promising and widely used strategy for constructing superstructures with well-defined nanostructures and diverse morphologies across multiple length scales. In this study, two homogeneous organohydrogels with distinct appearances were constructed by simply mixing polyoxometalate (phosphomolybdic acid, HPMo) and a double-tailed zwitterionic quaternary ammonium amphiphile in a binary solvent of water and dimethyl sulfoxide (DMSO). The delicate balance between electrostatic attraction and repulsion of anionic HPMo clusters and zwitterionic structures drove them to co-assemble into homogeneous organohydrogels with diverse microstructures. Notably, the morphologies of the organohydrogels, including unilamellar vesicles, onion-like vesicles, and spherical aggregates, can be controlled by adjusting the ionic interactions between the zwitterionic amphiphiles and phosphomolybdic acid clusters. Furthermore, we observed an organohydrogel fabricated with densely stacked onion-like structures (multilamellar vesicles) consisting of more than a dozen layers at certain proportions. Additionally, the relationships between the self-assembled architectures and the intermolecular interactions among the polyoxometalate, zwitterionic amphiphile, and solvent molecules were elucidated. This study offers valuable insights into the mechanisms of polyoxometalate-zwitterionic amphiphile co-assembly, which are essential for the development of materials with specific structures and emerging functionalities. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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11 pages, 514 KiB

Open AccessFeature PaperArticle

Quantifying the Hydrophobic Effect per CF₂ Moiety from Adsorption of Fluorinated Alcohols at the Water/Oil Interface

by Boyan Peychev, Dimitrinka Arabadzhieva, Ivan L. Minkov, Elena Mileva and Radomir I. Slavchov

Molecules 2024, 29(7), 1421; https://doi.org/10.3390/molecules29071421 - 22 Mar 2024

Viewed by 680

Abstract

Amphiphilic fluorocarbon substances are a trending topic of research due to their wide range of applications accompanied by an alarming environmental and health impact. In order to predict their fate in the environment, use them more economically, develop new water treatment methods, etc., a better understanding of their physicochemical behavior is required. Their hydrophobicity in water/oil systems is particularly sensitive to one key thermodynamic parameter: the free energy of transfer of a perfluoromethylene group from oil to water. However, for the –CF₂– moiety, the transfer energy values reported in the literature vary by more than ±25%. Due to the exponential relationship between this energy and the adsorption constants or the partition coefficients, such an uncertainty can lead to orders of magnitude error in the predicted distribution of fluorinated species. We address this problem by presenting an experimental determination of the hydrophobic effect of a –CF₂– moiety with a greater certainty than currently available. The transfer energy is determined by measuring the interfacial tension of water|hexane for aqueous solutions of short-chained fluorotelomer alcohols. The obtained results for the free energy of transfer of a –CF₂– moiety from oil to water are

1.68 \pm 0.02 \times R T_{0}

1.75 \pm 0.02 \times R T_{0}

, and

1.88 \pm 0.02 \times R T_{0}

at 288.15 K, 293.15 K, and 303.15 K, respectively. Full article

(This article belongs to the Special Issue Amphiphilic Molecules, Interfaces and Colloids)

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