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Recent Advances in Green Solvents II
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Recent Advances in Green Solvents II

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

Deadline for manuscript submissions: 31 May 2024 | Viewed by 5183

Special Issue Editor

Dr. Reza Haghbakhsh

E-Mail Website
Guest Editor
1. Department of Chemical Engineering, Faculty of Engineering, University of Isfahan, Isfahan, Iran
2. Department of Chemistry, School of Science and Technology, NOVA University Lisbon, Caparica, Portugal
Interests: green solvents; green chemistry; deep eutectic solvents; ionic liquids; applied thermodynamics; phase equilibria; physical properties; energy
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In previous decades, various industries were mostly developed at the cost of environmental neglect, resulting in numerous environmental issues and, ultimately, a distressing crisis to the planet. Therefore, in the 21st century, governments and world organizations are trying to legislate sustainable development laws for industrial advances. “Green chemistry”, as a rather novel field of chemistry and chemical engineering, is one of the key routes to assist researchers in sustainable development. Among the most valuable assets of green chemistry are “green solvents”, which are the primary candidates to replace the workhorses of numerous industries, i.e., the conventional harmful solvents. In recent decades, green solvents have been studied intensively by scientists and researchers, and the number of published articles has been growing exponentially. The most important green solvents, such as supercritical fluids, ionic liquids, and deep eutectic solvents, have been investigated in various fields and for numerous applications, yet much remains unknown and there is great room for further investigations on this class of solvents. 
 
This Special Issue aims to publish the most recent advances in the interdisciplinary area of green solvents. All of the research and review articles dealing with fundamental as well as application-based studies on green solvents are welcome, including, for example, theoretical studies at a molecular scale, thermodynamic investigations covering the phase behavior and pure and mixture physical properties, as well as industrially minded endeavors such as separations, reactions, catalysis, chemical processes, bioprocesses, food science, pharmaceuticals, environmental engineering, and innovative techniques.

Dr. Reza Haghbakhsh
Guest Editor

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

  • green solvents (deep eutectic solvents, ionic liquids, and supercritical fluids)
  • theoretical and thermodynamic investigations
  • green processes
  • sustainable separations
  • reactions and catalysis
  • environmental chemistry
  • bioproducts and biofuels
  • sustainable foods and pharmaceuticals

Published Papers (5 papers)

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Research

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19 pages, 2114 KiB  
Article
Experimental and Machine-Learning-Assisted Design of Pharmaceutically Acceptable Deep Eutectic Solvents for the Solubility Improvement of Non-Selective COX Inhibitors Ibuprofen and Ketoprofen
by Piotr Cysewski, Tomasz Jeliński, Maciej Przybyłek, Anna Mai and Julia Kułak
Molecules 2024, 29(10), 2296; https://doi.org/10.3390/molecules29102296 - 14 May 2024
Viewed by 434
Abstract
Deep eutectic solvents (DESs) are commonly used in pharmaceutical applications as excellent solubilizers of active substances. This study investigated the tuning of ibuprofen and ketoprofen solubility utilizing DESs containing choline chloride or betaine as hydrogen bond acceptors and various polyols (ethylene glycol, diethylene [...] Read more.
Deep eutectic solvents (DESs) are commonly used in pharmaceutical applications as excellent solubilizers of active substances. This study investigated the tuning of ibuprofen and ketoprofen solubility utilizing DESs containing choline chloride or betaine as hydrogen bond acceptors and various polyols (ethylene glycol, diethylene glycol, triethylene glycol, glycerol, 1,2-propanediol, 1,3-butanediol) as hydrogen bond donors. Experimental solubility data were collected for all DES systems. A machine learning model was developed using COSMO-RS molecular descriptors to predict solubility. All studied DESs exhibited a cosolvency effect, increasing drug solubility at modest concentrations of water. The model accurately predicted solubility for ibuprofen, ketoprofen, and related analogs (flurbiprofen, felbinac, phenylacetic acid, diphenylacetic acid). A machine learning approach utilizing COSMO-RS descriptors enables the rational design and solubility prediction of DES formulations for improved pharmaceutical applications. Full article
(This article belongs to the Special Issue Recent Advances in Green Solvents II)
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19 pages, 3583 KiB  
Article
Green and Efficient Extraction of Phenolic Components from Plants with Supramolecular Solvents: Experimental and Theoretical Studies
by Bo-Hou Xia, Zhi-Lu Yu, Yu-Ai Lu, Shi-Jun Liu, Ya-Mei Li, Ming-Xia Xie and Li-Mei Lin
Molecules 2024, 29(9), 2067; https://doi.org/10.3390/molecules29092067 - 30 Apr 2024
Viewed by 524
Abstract
The supramolecular solvent (SUPRAS) has garnered significant attention as an innovative, efficient, and environmentally friendly solvent for the effective extraction and separation of bioactive compounds from natural resources. However, research on the use of a SUPRAS for the extraction of phenolic compounds from [...] Read more.
The supramolecular solvent (SUPRAS) has garnered significant attention as an innovative, efficient, and environmentally friendly solvent for the effective extraction and separation of bioactive compounds from natural resources. However, research on the use of a SUPRAS for the extraction of phenolic compounds from plants, which are highly valued in food products due to their exceptional antioxidant properties, remains scarce. The present study developed a green, ultra-sound-assisted SUPRAS method for the simultaneous determination of three phenolic acids in Prunella vulgaris using high-performance liquid chromatography (HPLC). The experimental parameters were meticulously optimized. The efficiency and antioxidant properties of the phenolic compounds obtained using different extraction methods were also compared. Under optimal conditions, the extraction efficiency of the SUPRAS, prepared with octanoic acid reverse micelles dispersed in ethanol–water, significantly exceeded that of conventional organic solvents. Moreover, the SUPRAS method demonstrated greater antioxidant capacity. Confocal laser scanning microscopy (CLSM) images revealed the spherical droplet structure of the SUPRAS, characterized by a well-defined circular fluorescence position, which coincided with the position of the phenolic acids. The phenolic acids were encapsulated within the SUPRAS droplets, indicating their efficient extraction capacity. Furthermore, molecular dynamics simulations combined with CLSM supported the proposed method’s mechanism and theoretically demonstrated the superior extraction performance of the SUPRAS. In contrast to conventional methods, the higher extraction efficiency of the SUPRAS can be attributed to the larger solvent contact surface area, the formation of more types of hydrogen bonds between the extractants and the supramolecular solvents, and stronger, more stable interaction forces. The results of the theoretical studies corroborate the experimental outcomes. Full article
(This article belongs to the Special Issue Recent Advances in Green Solvents II)
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15 pages, 5516 KiB  
Article
Deep Eutectic Solvents as Agents for Improving the Solubility of Edaravone: Experimental and Theoretical Considerations
by Tomasz Jeliński, Maciej Przybyłek, Magdalena Mianowana, Kinga Misiak and Piotr Cysewski
Molecules 2024, 29(6), 1261; https://doi.org/10.3390/molecules29061261 - 12 Mar 2024
Cited by 1 | Viewed by 777
Abstract
In this study, both practical and theoretical aspects of the solubility of edaravone (EDA) in Deep Eutectic Solvents (DESs) were considered. The solubility of edaravone in some media, including water, can be limited, which creates the need for new efficient and environmentally safe [...] Read more.
In this study, both practical and theoretical aspects of the solubility of edaravone (EDA) in Deep Eutectic Solvents (DESs) were considered. The solubility of edaravone in some media, including water, can be limited, which creates the need for new efficient and environmentally safe solvents. The solubility of EDA was measured spectrophotometrically and the complex intermolecular interactions within the systems were studied with the COSMO-RS framework. Of the four studied DES systems, three outperformed the most efficient classical organic solvent, namely dichloromethane, with the DES comprising choline chloride and triethylene glycol, acting as hydrogen bond donor (HBD), in a 1:2 molar proportion yielding the highest solubility of EDA. Interestingly, the addition of a specific amount of water further increased EDA solubility. Theoretical analysis revealed that in pure water or solutions with high water content, EDA stacking is responsible for self-aggregation and lower solubility. On the other hand, the presence of HBDs leads to the formation of intermolecular clusters with EDA, reducing self-aggregation. However, in the presence of a stoichiometric amount of water, a three-molecular EDA–HBD–water complex is formed, which explains why water can also act as a co-solvent. The high probability of formation of this type of complexes is related to the high affinity of the components, which exceeds all other possible complexes. Full article
(This article belongs to the Special Issue Recent Advances in Green Solvents II)
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22 pages, 3425 KiB  
Article
Juçara Fruit (Euterpe Edulis Martius) Valorization Combining Emergent Extraction Technologies and Aqueous Solutions of Alkanediols
by Bruna P. Soares, Ana M. Ferreira, Marina Justi, Luiz Gustavo Gonçalves Rodrigues, J. Vladimir Oliveira, Simão P. Pinho and João A. P. Coutinho
Molecules 2023, 28(4), 1607; https://doi.org/10.3390/molecules28041607 - 7 Feb 2023
Cited by 2 | Viewed by 2003
Abstract
Anthocyanins from juçara fruits were extracted by pressurized liquid extraction (PLE) or ultrasound-assisted extraction (UAE), using aqueous solutions of 1,2-alkanediols and glycerol ethers as biobased solvents. The PLE (100 bar, 13 min, 1 mL/min flow rate) in the optimal extraction conditions originated 23.1 [...] Read more.
Anthocyanins from juçara fruits were extracted by pressurized liquid extraction (PLE) or ultrasound-assisted extraction (UAE), using aqueous solutions of 1,2-alkanediols and glycerol ethers as biobased solvents. The PLE (100 bar, 13 min, 1 mL/min flow rate) in the optimal extraction conditions originated 23.1 mganthocyanins·gdry biomass−1. On the other hand, the UAE was 10 min long, and the optimal conditions using 1,2-propanediol were 42.6 wt%, 160 W, and pH 7.0, leading to 50 mganthocyanins·gdry biomass−1. Extractions at the UAE optimized conditions, with aqueous solutions of five different 1,2-alkanediols and three glycerol ethers were performed, and compared to water and ethanolic extracts. The biobased solvent solutions presented anthocyanin yields up to 33% higher than water, and were shown to be as efficient as ethanol/water, but generated extracts with higher antioxidant capacity. The anthocyanin-rich extract of juçara, obtained with 1,2-propanediol, was used in the production of a natural soap and incorporated into a cream, showing that the addition of the juçara extract resulted in an antioxidant capacity in both products. Full article
(This article belongs to the Special Issue Recent Advances in Green Solvents II)
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Review

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12 pages, 253 KiB  
Review
Utilizing Deep Eutectic Solvents in the Recycle, Recovery, Purification and Miscellaneous Uses of Rare Earth Elements
by Francisco Jose Alguacil
Molecules 2024, 29(6), 1356; https://doi.org/10.3390/molecules29061356 - 19 Mar 2024
Viewed by 978
Abstract
The boosted interest in using rare earth elements (REEs) in modern technologies has also increased the necessity of their recovery from various sources, including raw materials and wastes. Though hydrometallurgy plays a key role in these recovery processes, some drawbacks (apparent or not) [...] Read more.
The boosted interest in using rare earth elements (REEs) in modern technologies has also increased the necessity of their recovery from various sources, including raw materials and wastes. Though hydrometallurgy plays a key role in these recovery processes, some drawbacks (apparent or not) of these processes (including the use of aggressive mineral acids, harmful extractants, and diluents, etc.) have led to the development of an environmental friendship subclass named solvometallurgy, in which non-aqueous solvents substituted to the aqueous media of the hydrometallurgical processing. Together with ionic liquids (ILs), the non-aqueous solvents chosen for these usages are the chemicals known as deep eutectic solvents (DEEs). The utilization of DEEs included the leaching of REEs from the different sources containing them and also in the separation-purification steps necessary for yielding these elements, normally oxides or salts, in the most purified form. This work reviewed the most recent literature (2023 year) about using deep eutectic solvents to recover REEs from various sources and coupling these two (DESs and REEs) to derive compounds to be used in other fields. Full article
(This article belongs to the Special Issue Recent Advances in Green Solvents II)
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