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Advances in Deep Eutectic Solvents
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Advances in Deep Eutectic Solvents

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

Deadline for manuscript submissions: closed (31 October 2024) | Viewed by 16750

Special Issue Editors

Dr. Zhijian Tan

E-Mail Website
Guest Editor
Institute of Bast Fiber Crops and Center of Southern Economic Crops, Chinese Academy of Agricultural Sciences, Changsha 410205, China
Interests: bioactive ingredients in food resources; food packaging; food preservation; biodegradable materials; green solvents; deep eutectic solvents; ionic liquids; bio-based solvents; solid–liquid extraction; liquid–liquid extraction
Special Issues, Collections and Topics in MDPI journals
Dr. Hongye Cheng

E-Mail Website
Guest Editor
School of Chemical Engineering, East China University of Science and Technology, Shanghai, China
Interests: deep eutectic solvent; ionic liquid; extraction and separation; reactive extraction; solvent screening; molecular simulation
Dr. Baokun Tang

E-Mail Website
Guest Editor
College of Pharmaceutical Sciences, Hebei University, Baoding 071002, China
Interests: deep eutectic solvents; ionic liquid; extraction and separation; adsorbent; fluorescence; bioactive compounds

Special Issue Information

Dear Colleagues,

Recently, deep eutectic solvents (DESs) have been considered as green solvents owing to their nonvolatility, easy preparation, adjustable structures, low biotoxicity, and high biodegradability. DESs have been used as excellent alternatives to conventional ionic liquids and volatile organic solvents in various applications, such as extraction, absorption, reaction, electrochemistry, materials synthesis, thermodynamics, drug delivery, energy storage, photoelectricity, biotechnology, sensors, and so on. This Special Issue, "Advances in Deep eutectic solvents", aims to collect and disseminate some of the most significant and recent contributions in the field of deep eutectic solvents.

For this Special Issue on “Advances in Deep Eutectic Solvents”, we would like to invite researchers to submit original articles and review articles that introduce the latest progress in DESs. Topics of interest include, but are not limited to:

•    Physical and chemical properties of DESs;
•    Extraction (or adsorption) of bioactive molecules using DESs;
•    Gas absorption and separation using DESs;
•    Catalysis and reaction using DESs;
•    Biomass pretreatment using DESs;
•    Novel materials preparation using DESs;
•    Drug delivery using DESs;
•    Cell, DNA, RNA, etc., biotechnologies based on DESs;
•    Detection sensors based on DESs;
•    Theoretical calculation based on DESs.

Prof. Dr. Zhijian Tan
Dr. Hongye Cheng
Dr. Baokun Tang
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
  • DES-based function materials
  • extraction
  • purification
  • reaction
  • separation
  • absorption
  • theoretical calculation

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Published Papers (8 papers)

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Research

9 pages, 2477 KiB  
Article
ZnCl2-Based Deep Eutectic Solvent as Solvent-Catalyst in the Michael Addition Reaction of Pyrrole to Maleimide
by Abelardo Gutiérrez-Hernández, Fátima M. Soto-Suárez, Arlette Richaud, Francisco Méndez and Claudia Araceli Contreras-Celedón
Molecules 2024, 29(22), 5381; https://doi.org/10.3390/molecules29225381 - 15 Nov 2024
Viewed by 302
Abstract
The use of deep eutectic solvents (DESs) as catalysts presents indisputable advantages, for example, their simplicity of preparation, high biodegradability, and recyclability, as well as zero toxicity and their effectiveness as environmentally friendly reaction media. However, aspects related to their reactivity and catalytic [...] Read more.
The use of deep eutectic solvents (DESs) as catalysts presents indisputable advantages, for example, their simplicity of preparation, high biodegradability, and recyclability, as well as zero toxicity and their effectiveness as environmentally friendly reaction media. However, aspects related to their reactivity and catalytic activity are still unclear. In this work, we explore the versatility of ChCl/ZnCl2 DES in the formation of C-C bonds through the Michael-type addition of pyrrole to maleimide, where ChCl/ZnCl2 DES leads to catalysis and chelation of the substrates, thus describing a recommended method for the construction of C-C bonds with high atomic economy. We describe experimental and theoretical aspects that explain the ability of ChCl/ZnCl2 DES in the presence of water to act as a catalyst in the formation of C-C bonds between pyrrole and maleimide. The potential energy surface showed that the ChCl and the zinc-zincate species 2ZnCl2·3H2O, formed by the interaction between zinc chloride and water, decrease the relative free Gibbs energy values for all the species involved in the reaction mechanism (TSs, intermediates, product), favoring the kinetics and thermodynamics of the Michael addition. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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6 pages, 3115 KiB  
Communication
The Reaction between K2CO3 and Ethylene Glycol in Deep Eutectic Solvents
by Yi Zhou, Mingzhe Chen, Xueling Dong and Dezhong Yang
Molecules 2024, 29(17), 4113; https://doi.org/10.3390/molecules29174113 - 30 Aug 2024
Viewed by 678
Abstract
Understanding intermolecular interactions is important for the design of deep eutectic solvents. Herein, potassium carbonate (K2CO3) and ethylene glycol (EG) are used to form deep eutectic solvents. The interactions between K2CO3 and EG are studied using [...] Read more.
Understanding intermolecular interactions is important for the design of deep eutectic solvents. Herein, potassium carbonate (K2CO3) and ethylene glycol (EG) are used to form deep eutectic solvents. The interactions between K2CO3 and EG are studied using nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectra. Interestingly, the interaction results indicate that the carbonate anion CO32− can react with EG to form EG-based organic carbonate, which can occur even at room temperature. The possible reaction steps between K2CO3 and EG are presented. As K2CO3 can be prepared from CO2 and KOH, the findings of this work may provide a promising strategy for CO2 capture and conversion. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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18 pages, 3181 KiB  
Article
High-Temperature Hydrothermal Extraction of Phenolic Compounds from Brewer’s Spent Grain and Malt Dust Biomass Using Natural Deep Eutectic Solvents
by Dries Bleus, Heike Blockx, Emma Gesquiere, Peter Adriaensens, Pieter Samyn, Wouter Marchal and Dries Vandamme
Molecules 2024, 29(9), 1983; https://doi.org/10.3390/molecules29091983 - 25 Apr 2024
Viewed by 1383
Abstract
Aligned with the EU Sustainable Development Goals 2030 (EU SDG2030), extensive research is dedicated to enhancing the sustainable use of biomass waste for the extraction of pharmaceutical and nutritional compounds, such as (poly-)phenolic compounds (PC). This study proposes an innovative one-step hydrothermal extraction [...] Read more.
Aligned with the EU Sustainable Development Goals 2030 (EU SDG2030), extensive research is dedicated to enhancing the sustainable use of biomass waste for the extraction of pharmaceutical and nutritional compounds, such as (poly-)phenolic compounds (PC). This study proposes an innovative one-step hydrothermal extraction (HTE) at a high temperature (120 °C), utilizing environmentally friendly acidic natural deep eutectic solvents (NADESs) to replace conventional harmful pre-treatment chemicals and organic solvents. Brewer’s spent grain (BSG) and novel malt dust (MD) biomass sources, both obtained from beer production, were characterized and studied for their potential as PC sources. HTE, paired with mild acidic malic acid/choline chloride (MA) NADES, was compared against conventional (heated and stirred maceration) and modern (microwave-assisted extraction; MAE) state-of-the-art extraction methods. The quantification of key PC in BSG and MD using liquid chromatography (HPLC) indicated that the combination of elevated temperatures and acidic NADES could provide significant improvements in PC extraction yields ranging from 251% (MD-MAC-MA: 29.3 µg/g; MD-HTE-MA: 103 µg/g) to 381% (BSG-MAC-MA: 78 µg/g; BSG-HTE-MA: 375 µg/g). The superior extraction capacity of MA NADES over non-acidic NADES (glycerol/choline chloride) and a traditional organic solvent mixture (acetone/H2O) could be attributed to in situ acid-catalysed pre-treatment facilitating the release of bound PC from lignin–hemicellulose structures. Qualitative 13C-NMR and pyro-GC-MS analysis was used to verify lignin–hemicellulose breakdown during extraction and the impact of high-temperature MA NADES extraction on the lignin–hemicellulose structure. This in situ acid NADES-catalysed high-temperature pre-treatment during PC extraction offers a potential green pre-treatment for use in cascade valorisation strategies (e.g., lignin valorisation), enabling more intensive usage of available biomass waste stream resources. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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16 pages, 4153 KiB  
Article
Improved Stability and Catalytic Efficiency of ω-Transaminase in Aqueous Mixture of Deep Eutectic Solvents
by Hongpeng Wang, Mercy Vimbai Masuku, Yachen Tao, Jiayao Yang, Yi Kuang, Changjiang Lyu, Jun Huang and Shengxiang Yang
Molecules 2023, 28(9), 3895; https://doi.org/10.3390/molecules28093895 - 5 May 2023
Cited by 2 | Viewed by 1658
Abstract
The efficient biosynthesis of chiral amines at an industrial scale to meet the high demand from industries that require chiral amines as precursors is challenging due to the poor stability and low catalytic efficiency of ω-transaminases (ω-TAs). Herein, this study adopted a green [...] Read more.
The efficient biosynthesis of chiral amines at an industrial scale to meet the high demand from industries that require chiral amines as precursors is challenging due to the poor stability and low catalytic efficiency of ω-transaminases (ω-TAs). Herein, this study adopted a green and efficient solvent engineering method to explore the effects of various aqueous solutions of deep eutectic solvents (DESs) as cosolvents on the catalytic efficiency and stability of ω-TA. Binary- and ternary-based DESs were used as cosolvents in enhancing the catalytic activity and stability of a ω-TA variant from Aspergillus terreus (E133A). The enzyme exhibited a higher catalytic activity in a ternary-based DES that was 2.4-fold higher than in conventional buffer. Moreover, the thermal stability was enhanced by a magnitude of 2.7, with an improvement in storage stability. Molecular docking studies illustrated that the most potent DES established strong hydrogen bond interactions with the enzyme’s amino acid, which enhanced the catalytic efficiency and improved the stability of the ω-TA. Molecular docking is essential in designing DESs for a specific enzyme. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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13 pages, 2126 KiB  
Article
Pt2CeO2 Heterojunction Supported on Multiwalled Carbon Nanotubes for Robust Electrocatalytic Oxidation of Methanol
by Pingping Yang, Xuejiao Wei, Li Zhang, Shiming Dong, Wenting Cao, Dong Ma and Yuejun Ouyang
Molecules 2023, 28(7), 2995; https://doi.org/10.3390/molecules28072995 - 27 Mar 2023
Cited by 2 | Viewed by 1553
Abstract
Herein, we prepared Pt2CeO2 heterojunction nanocluster (HJNS) on multiwalled carbon nanotubes (MWCNTs) in deep eutectic solvents (DESs) which is a special class of ionic liquids. The catalyst was then heat-treated at 400 °C in N2 (refer to Pt2 [...] Read more.
Herein, we prepared Pt2CeO2 heterojunction nanocluster (HJNS) on multiwalled carbon nanotubes (MWCNTs) in deep eutectic solvents (DESs) which is a special class of ionic liquids. The catalyst was then heat-treated at 400 °C in N2 (refer to Pt2CeO2/CNTs-400). The Pt2CeO2/CNTs-400 catalyst showed remarkably improved electrocatalytic performance towards methanol oxidation reaction (MOR) (839.1 mA mgPt−1) compared to Pt2CeO2/CNTs-500 (620.3 mA mgPt−1), Pt2CeO2/CNTs-300 (459.2 mA mgPt−1), Pt2CeO2/CNTs (641.6 mAmg−1) (the catalyst which has not been heat-treated) and commercial Pt/C (229.9 mAmg−1). Additionally, the Pt2CeO2/CNTs-400 catalyst also showed better CO poisoning resistance (onset potential: 0.47 V) compared to Pt2CeO2/CNTs (0.56 V) and commercial Pt/C (0.58 V). The improved performance of Pt2CeO2/CNTs-400 catalyst is attributed to the addition of appropriate CeO2, which changed the electronic state around the Pt atoms, lowered the d-band of Pt atoms, formed more Ce-O-Pt bonds acting as new active sites, affected the adsorption of toxic intermediates and weakened the dissolution of Pt; on the other hand, with the assistance of thermal treatment at 400 °C, the obtained Pt2CeO2 HJNS expose more new active sites at the interface between Pt and CeO2 to enhance the electrochemical active surface area (ECSA) and the dehydrogenation process of MOR. Thirdly, DES is beneficial to the increase of the effective component Pt(0) in the carbonization process. The study shows a new way to construct high-performance Pt-CeO2 catalyst for the direct methanol fuel cell (DMFC). Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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10 pages, 1382 KiB  
Article
Separation and Purification of Astragalus membranaceus Polysaccharides by Deep Eutectic Solvents-Based Aqueous Two-Phase System
by Bangfu Liu and Zhijian Tan
Molecules 2022, 27(16), 5288; https://doi.org/10.3390/molecules27165288 - 19 Aug 2022
Cited by 14 | Viewed by 2792
Abstract
(1) Background: Aqueous two-phase systems (ATPSs) have been widely used in the separation and purification of bioactive substances in recent years. (2) Methods: In this study, deep eutectic solvents (DESs)-based ATPSs were employed for the extraction and separation of Astragalus membranaceus polysaccharides (AMP). [...] Read more.
(1) Background: Aqueous two-phase systems (ATPSs) have been widely used in the separation and purification of bioactive substances in recent years. (2) Methods: In this study, deep eutectic solvents (DESs)-based ATPSs were employed for the extraction and separation of Astragalus membranaceus polysaccharides (AMP). The optimal DES (choline chloride:urea = 1:1) was first screened to extract AMP, and the effect of DES concentration, solid–liquid ratio, pH, extraction temperature, and extraction time on the extraction yield of AMP were investigated. (3) Results: The maximum extraction yield was 141.11 mg/g under the optimum conditions. AMP was then preliminarily purified by ATPS, to further realize the recycling and reuse of DES. The effect of type of salts, salt concentration, and extraction temperature on extraction efficiency was investigated. The extraction efficiency was 97.85% for AMP under the optimum ATPS conditions. Finally, the obtained AMP was studied by molecular weight determination, infrared spectroscopy analysis, and monosaccharide composition analysis. (4) Conclusions: This ATPS extraction based on DESs is simple, environmentally friendly, low-cost, and has high extraction efficiency, which provides new ideas for the extraction of plant polysaccharides and other bioactive compounds. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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17 pages, 1977 KiB  
Article
Separation of Benzene and Cyclohexane Using Eutectic Solvents with Aromatic Structure
by Mohamed K. Hadj-Kali, M. Zulhaziman M. Salleh, Irfan Wazeer, Ahmad Alhadid and Sarwono Mulyono
Molecules 2022, 27(13), 4041; https://doi.org/10.3390/molecules27134041 - 23 Jun 2022
Cited by 7 | Viewed by 2412
Abstract
The separation of benzene and cyclohexane is a challenging process in the petrochemical industry, mainly because of their close boiling points. Extractive separation of the benzene-cyclohexane mixture has been shown to be feasible, but it is important to find solvents with good extractive [...] Read more.
The separation of benzene and cyclohexane is a challenging process in the petrochemical industry, mainly because of their close boiling points. Extractive separation of the benzene-cyclohexane mixture has been shown to be feasible, but it is important to find solvents with good extractive performance. In this work, 23 eutectic solvents (ESs) containing aromatic components were screened using the predictive COSMO-RS and their respective performance was compared with other solvents. The screening results were validated with experimental work in which the liquid–liquid equilibria of the three preselected ESs were studied with benzene and cyclohexane at 298.5 K and 101.325 kPa, with benzene concentrations in the feed ranging from 10 to 60 wt%. The performance of the ESs studied was compared with organic solvents, ionic liquids, and other ESs reported in the literature. This work demonstrates the potential for improved extractive separation of the benzene-cyclohexane mixture by using ESs with aromatic moieties. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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12 pages, 1378 KiB  
Article
Green and Efficient Extraction of Polysaccharide and Ginsenoside from American Ginseng (Panax quinquefolius L.) by Deep Eutectic Solvent Extraction and Aqueous Two-Phase System
by Rong-Rong Zhou, Jian-Hua Huang, Dan He, Zi-Yang Yi, Di Zhao, Zhao Liu, Shui-Han Zhang and Lu-Qi Huang
Molecules 2022, 27(10), 3132; https://doi.org/10.3390/molecules27103132 - 13 May 2022
Cited by 24 | Viewed by 4133
Abstract
In this study, a green and effective extraction method was proposed to extract two main compounds, ginsenosides and polysaccharides, from American ginseng by combining deep eutectic solvents (DESs) with aqueous two-phase systems. The factors of type of DESs, water content in DESs, the [...] Read more.
In this study, a green and effective extraction method was proposed to extract two main compounds, ginsenosides and polysaccharides, from American ginseng by combining deep eutectic solvents (DESs) with aqueous two-phase systems. The factors of type of DESs, water content in DESs, the solid–liquid ratio, extraction temperature, and extraction time were studied in the solid–liquid extraction. Then, the aqueous two-phase system (DESs-ethylene oxide–propylene oxide (EOPO)) and salty solution exchange (EOPO-salty solution) was applied for the purification of polysaccharides. The content of the polysaccharides and ginsenosides were analyzed by the anthrone–sulfuric acid method and HPLC method, which showed that the extraction efficiency of deep eutectic solvents (DESs) was better than conventional methods. Moreover, the antioxidant activities of ginseng polysaccharides and their cytotoxicity were further assayed. The advantages of the current study are that, throughout the whole extraction process, we avoided the usage of an organic reagent. Furthermore, the separated green solvent DESs and EOPO could be recovered and reused for a next cycle. Thus, this study proposed a new, green and recyclable extraction method for extracting ginsenosides and polysaccharides from American ginseng. Full article
(This article belongs to the Special Issue Advances in Deep Eutectic Solvents)
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