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Breakthrough Developments in Fundamental Studies and Applications of Deep Eutectic...
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Breakthrough Developments in Fundamental Studies and Applications of Deep Eutectic Systems

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

Deadline for manuscript submissions: closed (15 February 2023) | Viewed by 17834

Special Issue Editors

Dr. Ana Rita C. Duarte

E-Mail Website
Guest Editor
Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa, Caparica, Portugal
Interests: supercritical particle; supercritical fluids; eutectic systems
Dr. Alexandre Paiva

E-Mail Website
Guest Editor
Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa, Caparica, Portugal
Interests: subcritical water; supercritical fluids; biocatalysis and deep eutectic solvents

Special Issue Information

Dear Colleagues,

This Special Issue is related to The 2nd International Meeting on Deep Eutectic Systems, which will be the second event of a fruitful series of meetings where scientists, students, and industry partners can discuss current developments and innovations based on the extraordinary properties of deep eutectic systems (DES). The conference will be hosted online from the 15-17th June 2021.

DES have shown great promise for application in several different areas, such as chemistry, electrochemistry, biotechnology, health and pharma, cosmetics or the paper industry. Therefore, scientific research in this field assumes huge relevance, and we can expect a significant impact in numerous sectors which can change the course of society, economy, and industry toward a greener and more sustainable future. The conference will address the following topics: extraction and separation, fundamental properties, biotech, materials, and energy and electrochemistry.

Participants of the symposium, as well as all researchers working in the field, are cordially invited to contribute original research papers or reviews to this Special Issue of Molecules, which report on any of these topics.

Dr. Ana Rita C. Duarte
Dr. Alexandre Paiva
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Molecules is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • deep eutectic solvents
  • natural deep eutectic solvents
  • electrochemistry
  • materials
  • pharmaceutics
  • cosmetics
  • extraction and separation
  • biotechnology
  • energy
  • thermodynamics

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Published Papers (4 papers)

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Research

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19 pages, 1316 KiB  
Article
Viscosity Investigations on the Binary Systems of (1 ChCl:2 Ethylene Glycol) DES and Methanol or Ethanol
by Reza Haghbakhsh, Ana Rita C. Duarte and Sona Raeissi
Molecules 2021, 26(18), 5513; https://doi.org/10.3390/molecules26185513 - 10 Sep 2021
Cited by 14 | Viewed by 2639
Abstract
In this study, the viscosity behavior of two mixtures of Ethaline (1 ChCl:2 ethylene glycol) with either methanol or ethanol were investigated over the temperature range of 283.15–333.15 K at atmospheric pressure. The measured viscosities of neat Ethaline, methanol, and ethanol showed reliable [...] Read more.
In this study, the viscosity behavior of two mixtures of Ethaline (1 ChCl:2 ethylene glycol) with either methanol or ethanol were investigated over the temperature range of 283.15–333.15 K at atmospheric pressure. The measured viscosities of neat Ethaline, methanol, and ethanol showed reliable agreement with the corresponding reported literature values. The mixture viscosities were modeled by an Arrhenius-like model to determine the behavior of viscosity with respect to temperature. The data were also modeled by the four well-known mixture viscosity models of Grunberg–Nissan, Jouyban–Acree, McAllister, and Preferential Solvation. All of the model results were reliable, with the Jouyban–Acree and Preferential Solvation models showing the most accurate agreement with the experimental measurements. The Jones–Dole viscosity model was also investigated for the measured viscosities, and by analyzing the results of this model, strong interactions among Ethaline and the alcohol molecules were proposed for both systems. As a final analysis, viscosity deviations of the investigated systems were calculated to study the deviations of the viscosity behaviors with respect to ideal behavior. Both systems showed negative viscosity deviations at all of the investigated temperatures, with the negative values tending towards zero, and hence more ideal behavior, with increasing temperatures. Moreover, in order to correlate the calculated viscosity deviations, the Redlich–Kister model was successfully used for both systems and at each investigated temperature. Full article
(This article belongs to the Special Issue Breakthrough Developments in Fundamental Studies and Applications of Deep Eutectic Systems)
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18 pages, 2950 KiB  
Article
In Situ Water Quantification in Natural Deep Eutectic Solvents Using Portable Raman Spectroscopy
by Suha Elderderi, Laura Wils, Charlotte Leman-Loubière, Hugh J. Byrne, Igor Chourpa, Cécile Enguehard-Gueiffier, Emilie Munnier, Abdalla A. Elbashir, Leslie Boudesocque-Delaye and Franck Bonnier
Molecules 2021, 26(18), 5488; https://doi.org/10.3390/molecules26185488 - 9 Sep 2021
Cited by 7 | Viewed by 4570
Abstract
Raman spectroscopy is a label-free, non-destructive, non-invasive analytical tool that provides insight into the molecular composition of samples with minimum or no sample preparation. The increased availability of commercial portable Raman devices presents a potentially easy and convenient analytical solution for day-to-day analysis [...] Read more.
Raman spectroscopy is a label-free, non-destructive, non-invasive analytical tool that provides insight into the molecular composition of samples with minimum or no sample preparation. The increased availability of commercial portable Raman devices presents a potentially easy and convenient analytical solution for day-to-day analysis in laboratories and production lines. However, their performance for highly specific and sensitive analysis applications has not been extensively evaluated. This study performs a direct comparison of such a commercially available, portable Raman system, with a research grade Raman microscope system for the analysis of water content of Natural Deep Eutectic Solvents (NADES). NADES are renewable, biodegradable and easily tunable “green” solvents, outcompeting existing organic solvents for applications in extraction from biomass, biocatalysis, and nanoparticle synthesis. Water content in NADES is, however, a critical parameter, affecting their properties, optimal use and extraction efficiency. In the present study, portable Raman spectroscopy coupled with Partial Least Squares Regression (PLSR) is investigated for rapid determination of water content in NADES samples in situ, i.e., directly in glassware. Three NADES systems, namely Betaine Glycerol (BG), Choline Chloride Glycerol (CCG) and Glucose Glycerol (GG), containing a range of water concentrations between 0% (w/w) and 28.5% (w/w), were studied. The results are directly compared with previously published studies of the same systems, using a research grade Raman microscope. PLSR results demonstrate the reliability of the analysis, surrendering R2 values above 0.99. Root Mean Square Errors Prediction (RMSEP) of 0.6805%, 0.9859% and 1.2907% w/w were found for respectively unknown CCG, BG and GG samples using the portable device compared to 0.4715%, 0.3437% and 0.7409% w/w previously obtained by analysis in quartz cuvettes with a Raman confocal microscope. Despite the relatively higher values of RMSEP observed, the comparison of the percentage of relative errors in the predicted concentration highlights that, overall, the portable device delivers accuracy below 5%. Ultimately, it has been demonstrated that portable Raman spectroscopy enables accurate quantification of water in NADES directly through glass vials without the requirement for sample withdrawal. Such compact instruments provide solvent and consumable free analysis for rapid analysis directly in laboratories and for non-expert users. Portable Raman is a promising approach for high throughput monitoring of water content in NADES that can support the development of new analytical protocols in the field of green chemistry in research and development laboratories but also in the industry as a routine quality control tool. Full article
(This article belongs to the Special Issue Breakthrough Developments in Fundamental Studies and Applications of Deep Eutectic Systems)
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16 pages, 1959 KiB  
Article
Physicochemical Characterization and Simulation of the Solid–Liquid Equilibrium Phase Diagram of Terpene-Based Eutectic Solvent Systems
by Maha M. Abdallah, Simon Müller, Andrés González de Castilla, Pavel Gurikov, Ana A. Matias, Maria do Rosário Bronze and Naiara Fernández
Molecules 2021, 26(6), 1801; https://doi.org/10.3390/molecules26061801 - 23 Mar 2021
Cited by 24 | Viewed by 6403
Abstract
The characterization of terpene-based eutectic solvent systems is performed to describe their solid–liquid phase transitions. Physical properties are measured experimentally and compared to computed correlations for deep eutectic solvents (DES) and the percentage relative error er for the density, surface tension, and [...] Read more.
The characterization of terpene-based eutectic solvent systems is performed to describe their solid–liquid phase transitions. Physical properties are measured experimentally and compared to computed correlations for deep eutectic solvents (DES) and the percentage relative error er for the density, surface tension, and refractive index is obtained. The thermodynamic parameters, including the degradation, glass transition and crystallization temperatures, are measured using DSC and TGA. Based on these data, the solid–liquid equilibrium phase diagrams are calculated for the ideal case and predictions are made using the semi-predictive UNIFAC and the predictive COSMO RS models, the latter with two different parametrization levels. For each system, the ideal, experimental, and predicted eutectic points are obtained. The deviation from ideality is observed experimentally and using the thermodynamic models for Thymol:Borneol and Thymol:Camphor. In contrast, a negative deviation is observed only experimentally for Menthol:Borneol and Menthol:Camphor. Moreover, the chemical interactions are analyzed using FTIR and 1H-NMR to study the intermolecular hydrogen bonding in the systems. Full article
(This article belongs to the Special Issue Breakthrough Developments in Fundamental Studies and Applications of Deep Eutectic Systems)
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Review

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28 pages, 3634 KiB  
Review
Deep Eutectic Solvent-Mediated Electrocatalysts for Water Splitting
by Chenyun Zhang, Yongqi Fu, Wei Gao, Te Bai, Tianyi Cao, Jianjiao Jin and Bingwei Xin
Molecules 2022, 27(22), 8098; https://doi.org/10.3390/molecules27228098 - 21 Nov 2022
Cited by 15 | Viewed by 3165
Abstract
As green, safe, and cheap solvents, deep eutectic solvents (DESs) provide tremendous opportunities to open up attractive perspectives for electrocatalysis. In this review, the achievement of DESs in the preparation of catalysts for electrolytic water splitting is described in detail according to their [...] Read more.
As green, safe, and cheap solvents, deep eutectic solvents (DESs) provide tremendous opportunities to open up attractive perspectives for electrocatalysis. In this review, the achievement of DESs in the preparation of catalysts for electrolytic water splitting is described in detail according to their roles combined with our own work. DESs are generally employed as green media, templates, and electrolytes. A large number of hydrogen bonds in DESs result in supramolecular structures which have the ability to shape the morphologies of nanomaterials and then tune their performance. DESs can also serve as reactive reagents of metal electrocatalysts through directly participating in synthesis. Compared with conventional heteroatom sources, they have the advantages of high safety and designability. The “all-in-one” transformation strategy is expected to realize 100% atomic transformation of reactants. The aim of this review is to offer readers a deeper understanding on preparing DES-mediated electrocatalysts with higher performance for water splitting. Full article
(This article belongs to the Special Issue Breakthrough Developments in Fundamental Studies and Applications of Deep Eutectic Systems)
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