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Responsive Soft Materials Based on Biomolecules

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

Deadline for manuscript submissions: closed (30 April 2023) | Viewed by 11978

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Special Issue Editors

Dr. Anne-Laure Fameau

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Guest Editor

National Institute of French Agricultural and Environmental Research, INRAE, 59650 Villeneuve d’Asq, France
Interests: surfactant; self-assembly; foam; emulsion; lipid; responsive soft-materials

Prof. Dr. Yujun Feng

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Guest Editor

Polymer Research Institute, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, China
Interests: water-soluble polymers; smart polymers; wormlike micelles; oilfield chemistry; enhanced oil recovery
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Special Issue Information

Dear Colleagues,

A stimuli responsive system has its behavior modified by a stimulus which can change solution condition (pH, temperature and ionic strength) or by the application of an external field (light, magnetic and electric). The introduction of stimuli-responsive properties into soft matter systems is of significant interest in various research fields, including physical chemistry, materials chemistry, colloid science, nanotechnology, and biochemistry. These intelligent materials represent one of the most exciting and newly emerging areas of scientific interest with a wide range of potential applications. These smart materials are usually designed from synthetic molecules, most of which are harmful to the environment. However, biomolecules can also be used as building blocks to the design of responsive soft materials. By tuning the intermolecular and interparticle interactions, which govern the resulting physical properties of the supracolloidal structures, new pathways can be established to design responsive materials based on biomolecules. Thus, a wide range of responsive soft materials can be obtained: liquid foams, emulsions, gels, etc.

Dr. Anne-Laure Fameau
Prof. Dr. Yujun Feng
Guest Editors

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Keywords

responsive foam
responsive emulsion
responsive gels
responsive self-assembly
surfactant
biomacromolecules
proteins
lipid particles

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Published Papers (6 papers)

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Research

20 pages, 3433 KiB

Open AccessFeature PaperArticle

Aqueous Binary Mixtures of Stearic Acid and Its Hydroxylated Counterpart 12-Hydroxystearic Acid: Fine Tuning of the Lamellar/Micelle Threshold Temperature Transition and of the Micelle Shape

by Maëva Almeida, Daniel Dudzinski, Bastien Rousseau, Catherine Amiel, Sylvain Prévost, Fabrice Cousin and Clémence Le Coeur

Molecules 2023, 28(17), 6317; https://doi.org/10.3390/molecules28176317 - 29 Aug 2023

Cited by 3 | Viewed by 1207

Abstract

This study examines the structures of soft surfactant-based biomaterials which can be tuned by temperature. More precisely, investigated here is the behavior of stearic acid (SA) and 12-hydroxystearic acid (12-HSA) aqueous mixtures as a function of temperature and the 12-HSA/SA molar ratio (R). Whatever R is, the system exhibits a morphological transition at a given threshold temperature, from multilamellar self-assemblies at low temperature to small micelles at high temperature, as shown by a combination of transmittance measurements, Wide Angle X-ray diffraction (WAXS), small angle neutron scattering (SANS), and differential scanning calorimetry (DSC) experiments. The precise determination of the threshold temperature, which ranges between 20 °C and 50 °C depending on R, allows for the construction of the whole phase diagram of the system as a function of R. At high temperature, the micelles that are formed are oblate for pure SA solutions (R = 0) and prolate for pure 12-HSA solutions (R = 1). In the case of mixtures, there is a progressive continuous transition from oblate to prolate shapes when increasing R, with micelles that are almost purely spherical for R = 0.33. Full article

(This article belongs to the Special Issue Responsive Soft Materials Based on Biomolecules)

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24 pages, 3977 KiB

Open AccessArticle

Aqueous Binary Mixtures of Stearic Acid and Its Hydroxylated Counterpart 12-Hydroxystearic Acid: Cascade of Morphological Transitions at Room Temperature

by Maëva Almeida, Daniel Dudzinski, Catherine Amiel, Jean-Michel Guigner, Sylvain Prévost, Clémence Le Coeur and Fabrice Cousin

Molecules 2023, 28(11), 4336; https://doi.org/10.3390/molecules28114336 - 25 May 2023

Cited by 4 | Viewed by 2365

Abstract

Here, we describe the behavior of mixtures of stearic acid (SA) and its hydroxylated counterpart 12-hydroxystearic acid (12-HSA) in aqueous mixtures at room temperature as a function of the 12-HSA/SA mole ratio R. The morphologies of the self-assembled aggregates are obtained through a multi-structural approach that combines confocal and cryo-TEM microscopies with small-angle neutron scattering (SANS) and wide-angle X-ray scattering (WAXS) measurements, coupled with rheology measurements. Fatty acids are solubilized by an excess of ethanolamine counterions, so that their heads are negatively charged. A clear trend towards partitioning between the two types of fatty acids is observed, presumably driven by the favorable formation of a H-bond network between hydroxyl OH function on the 12th carbon. For all R, the self-assembled structures are locally lamellar, with bilayers composed of crystallized and strongly interdigitated fatty acids. At high R, multilamellar tubes are formed. The doping via a low amount of SA molecules slightly modifies the dimensions of the tubes and decreases the bilayer rigidity. The solutions have a gel-like behavior. At intermediate R, tubes coexist in solution with helical ribbons. At low R, local partitioning also occurs, and the architecture of the self-assemblies associates the two morphologies of the pure fatty acids systems: they are faceted objects with planar domains enriched in SA molecules, capped with curved domains enriched in 12-HSA molecules. The rigidity of the bilayers is strongly increased, as well their storage modulus. The solutions remain, however, viscous fluids in this regime. Full article

(This article belongs to the Special Issue Responsive Soft Materials Based on Biomolecules)

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14 pages, 2198 KiB

Open AccessArticle

Ultrastable and Responsive Foams Based on 10-Hydroxystearic Acid Soap for Spore Decontamination

by Carolina Dari, Fabrice Cousin, Clemence Le Coeur, Thomas Dubois, Thierry Benezech, Arnaud Saint-Jalmes and Anne-Laure Fameau

Molecules 2023, 28(11), 4295; https://doi.org/10.3390/molecules28114295 - 24 May 2023

Cited by 3 | Viewed by 1733

Abstract

Currently, there is renewed interest in using fatty acid soaps as surfactants. Hydroxylated fatty acids are specific fatty acids with a hydroxyl group in the alkyl chain, giving rise to chirality and specific surfactant properties. The most famous hydroxylated fatty acid is 12-hydroxystearic acid (12-HSA), which is widely used in industry and comes from castor oil. A very similar and new hydroxylated fatty acid, 10-hydroxystearic acid (10-HSA), can be easily obtained from oleic acid by using microorganisms. Here, we studied for the first time the self-assembly and foaming properties of R-10-HSA soap in an aqueous solution. A multiscale approach was used by combining microscopy techniques, small-angle neutron scattering, wide-angle X-ray scattering, rheology experiments, and surface tension measurements as a function of temperature. The behavior of R-10-HSA was systematically compared with that of 12-HSA soap. Although multilamellar micron-sized tubes were observed for both R-10-HSA and 12-HSA, the structure of the self-assemblies at the nanoscale was different, which is probably due to the fact that the 12-HSA solutions were racemic mixtures, while the 10-HSA solutions were obtained from a pure R enantiomer. We also demonstrated that stable foams based on R-10-HSA soap can be used for cleaning applications, by studying spore removal on model surfaces in static conditions via foam imbibition. Full article

(This article belongs to the Special Issue Responsive Soft Materials Based on Biomolecules)

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15 pages, 4861 KiB

Open AccessArticle

A Comparative Study on CO₂-Switchable Foams Stabilized by C₂₂- or C₁₈-Tailed Tertiary Amines

by Meiqing Liang, Xuezhi Zhao, Ji Wang and Yujun Feng

Molecules 2023, 28(6), 2567; https://doi.org/10.3390/molecules28062567 - 11 Mar 2023

Cited by 4 | Viewed by 1882

Abstract

The CO₂ aqueous foams stabilized by bioresource-derived ultra-long chain surfactants have demonstrated considerable promising application potential owing to their remarkable longevity. Nevertheless, existing research is still inadequate to establish the relationships among surfactant architecture, environmental factors, and foam properties. Herein, two cases of ultra-long chain tertiary amines with different tail lengths, N-erucamidopropyl-N,N-dimethylamine (UC₂₂AMPM) and N-oleicamidopropyl-N,N-dimethylamine (UC₁₈AMPM), were employed to fabricate CO₂ foams. The effect of temperature, pressure and salinity on the properties of two foam systems (i.e., foamability and foam stability) was compared using a high-temperature, high-pressure visualization foam meter. The continuous phase viscosity and liquid content for both samples were characterized using rheometry and FoamScan. The results showed that the increased concentrations or pressure enhanced the properties of both foam samples, but the increased scope for UC₂₂AMPM was more pronounced. By contrast, the foam stability for both cases was impaired with increasing salinity or temperature, but the UC₁₈AMPM sample is more sensitive to temperature and salinity, indicating the salt and temperature resistance of UC₁₈AMPM-CO₂ foams is weaker than those of the UC₂₂AMPM counterpart. These differences are associated with the longer hydrophobic chain of UC₂₂AMPM, which imparts a higher viscosity and lower surface tension to foams, resisting the adverse effects of temperature and salinity. Full article

(This article belongs to the Special Issue Responsive Soft Materials Based on Biomolecules)

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15 pages, 2709 KiB

Open AccessArticle

Decontamination of Spores on Model Stainless-Steel Surface by Using Foams Based on Alkyl Polyglucosides

by Carolina Dari, Heni Dallagi, Christine Faille, Thomas Dubois, Christelle Lemy, Maureen Deleplace, Marwan Abdallah, Cosmin Gruescu, Julie Beaucé, Thierry Benezech and Anne-Laure Fameau

Molecules 2023, 28(3), 936; https://doi.org/10.3390/molecules28030936 - 17 Jan 2023

Cited by 5 | Viewed by 2025

Abstract

In the food industry, the surfaces of processing equipment are considered to be major factors in the risk of food contamination. The cleaning process of solid surfaces is essential, but it requires a significant amount of water and chemicals. Herein, we report the use of foam flows based on alkyl polyglucosides (APGs) to remove spores of Bacillus subtilis on stainless-steel surfaces as the model-contaminated surface. Sodium dodecyl sulfate (SDS) was also studied as an anionic surfactant. Foams were characterized during flows by measuring the foam stability and the bubble size. The efficiency of spores’ removal was assessed by enumerations. We showed that foams based on APGs could remove efficiently the spores from the surfaces, but slightly less than foams based on SDS due to an effect of SDS itself on spores removal. The destabilization of the foams at the end of the process and the recovery of surfactant solutions were also evaluated by using filtration. Following a life cycle assessment (LCA) approach, we evaluated the impact of the foam flow on the global environmental footprint of the process. We showed significant environmental impact benefits with a reduction in water and energy consumption for foam cleaning. APGs are a good choice as surfactants as they decrease further the environmental impacts. Full article

(This article belongs to the Special Issue Responsive Soft Materials Based on Biomolecules)

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16 pages, 7974 KiB

Open AccessArticle

Thermoresponsive Dual-Structured Gel Emulsions Stabilized by Glycyrrhizic Acid Nanofibrils in Combination with Monoglyceride Crystals

by Jialing Chen, Qing Li, Ruijie Du, Xinke Yu, Zhili Wan and Xiaoquan Yang

Molecules 2022, 27(19), 6542; https://doi.org/10.3390/molecules27196542 - 3 Oct 2022

Cited by 5 | Viewed by 2144

Abstract

Responsive dual-structured emulsions and gel emulsions have attracted more and more attention due to their complex microstructures, on-demand responsive properties, and controlled release of active cargoes. In this work, the effect of monoglyceride (MG)-based oil phase structuring on the formation and stability, structural properties, and thermoresponsive and cargo release behavior of gel emulsions stabilized by glycyrrhizic acid (GA) nanofibrils were investigated. Owing to the formation of GA fibrillar networks in the aqueous phase and MG crystalline networks in the oil phase, a stable dual-structured gel emulsion can be successfully developed. The microstructure of the dual-structured gel emulsions largely depended on the concentration of MG in the oil phase. At low MG concentrations (1–2 wt%), the larger formed and lamellar MG crystals may pierce the interfacial fibrillar film, inducing the formation of partially coalesced droplets. In contrast, at high MG concentrations (4 wt% or above), the smaller MG crystals with enhanced interfacial activity can lead to the formation of a bilayer shell of GA nanofibrils and MG crystals, thus efficiently inhibiting the interfacial film damage and forming a jamming structure with homogeneously distributed small droplets. Compared to pure GA nanofibril gel emulsions, the GA−MG dual-structured gel emulsions showed significantly improved mechanical performance as well as good thermoresponsive behavior. Moreover, these stable GA−MG gel emulsions can be used as food-grade delivery vehicles for encapsulating and protecting hydrophobic and hydrophilic bioactive cargoes. They also have great potential as novel and efficient aroma delivery systems showing highly controlled volatile release. The dual-structured emulsion strategy is expected to broaden the applications of natural saponin GA-based gel emulsions in the food, pharmaceutical, and personal care industries. Full article

(This article belongs to the Special Issue Responsive Soft Materials Based on Biomolecules)

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