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Development and Application of Greener Organic Solvents

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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Green Materials".

Deadline for manuscript submissions: closed (20 October 2023) | Viewed by 19684

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Prof. Dr. Piotr Cysewski

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Department of Physical Chemistry, Pharmacy Faculty, Collegium Medicum of Bydgoszcz, Nicolaus Copernicus University in Toruń, Kurpińskiego 5, 85-950 Bydgoszcz, Poland
Interests: theoretical chemistry; in silico modeling; solution thermodynamics; new materials screening
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Special Issue Information

Dear Colleagues,

Solvent utilization is mandatory in a variety of chemical practices. Large volumes of solvents are used worldwide as reaction media and for purification purposes. A variety of formulations has turned attention to the related darker side of solvent use. The desire, necessity, and hope to avoid the use of toxic, flammable, or environmentally damaging solvents has provoked a shift toward a greener and more responsible attitude. Hence, it is not surprising that the Sustainable Chemistry concept became a hot topic and a rapidly growing and evolving discipline. Unfortunately, the selection of the greener solvents is not a straightforward task since it often requires a compromise between contradictory constraints. In general, several criteria are associated with the greening of hazardous solvents—namely, safety, occupational health, environment, quality, physicochemical properties, industrial constraints, and of course cost. For these reasons, a great deal of effort has been put into the development of this discipline in recent decades. This Special Issue is an attempt to collect examples of contemporary achievements in the field. The potential topics include but are not limited to:

Greener solvents: properties and applications;
Theoretical and practical aspects of structurally related solvents;
Strategies for the replacement of hazardous solvents with greener ones;
Regulations, restrictions, and legislations;
Classification and categorization of solvents with respect to properties or applications;
Present and future of green technologies in solvent development;
Supercritical fluid processing reaction systems;
Green solvents for organic reaction systems and industrial applications of green solvents;
Papers with new ideas, perspectives, personal experiences, and opinions toward the greener side of chemistry.

All these and other issues related to the environmental aspects of solvents will be welcome in this Special Issue. It is my great pleasure and privilege to invite you to contribute your research articles, communications, or reviews to this Special Issue.

Prof. Dr. Piotr Cysewski
Guest Editor

Manuscript Submission Information

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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. Materials 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 2600 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
solvent design
NADES
ionic liquids
bio-based solvents
solvent selection guides
green chemistry metrics
pharmaceutical synthesis

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Published Papers (7 papers)

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Research

15 pages, 5758 KiB

Open AccessArticle

Electrodeposition of Bi from Choline Chloride-Malonic Acid Deep Eutectic Solvent

by Xiaozhou Cao, Hao Wang, Tianrui Liu, Yuanyuan Shi and Xiangxin Xue

Materials 2023, 16(1), 415; https://doi.org/10.3390/ma16010415 - 1 Jan 2023

Cited by 7 | Viewed by 2896

Abstract

Deep eutectic solvent (DES) has been widely used in the field of metal electrodeposition as an economical and environmentally friendly green solvent. Metallic bismuth films were prepared by electrodeposition from choline chloride-malonic acid (ChCl-MA) deep eutectic solvent (DES) containing BiCl₃. Fourier transform infrared (FTIR) spectroscopy and Raman spectroscopy were used to study the structure of ChCl-MA-BiCl₃, and the results showed that Bi(III) was in the form of [BiCl₆]³⁻ ions. The viscosity of ChCl-MA-BiCl₃ ranges from 200 to 1200 mPa·s at temperatures from 363 K to 323 K. The conductivity of 0.01 M Bi(III) in ChCl–MA is 3.24 ms·cm⁻¹ at 363 K. The electrochemical behavior and electrodeposition of Bi(III) in DES were investigated by cyclic voltammetry (CV) and chronoamperometry. The results showed that the electrodeposition reaction was a quasi-reversible reaction controlled by the diffusion and the nucleation of bismuth was a three-dimensional instantaneous nucleation. The diffusion coefficient of Bi(III) in ChCl-MA was 1.84 × 10⁻⁹ cm²·s⁻¹. The electrodeposition product was observed by scanning electron microscopy (SEM), and the results showed that the deposition potential has a significant influence on the morphology of the bismuth film. X-ray photoelectron spectroscopy (XPS) shows that bismuth and bismuth oxides are present in the deposited film obtained by electrodeposition. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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17 pages, 2215 KiB

Open AccessArticle

Solubilization and Thermodynamic Analysis of Isotretinoin in Eleven Different Green Solvents at Different Temperatures

by Faiyaz Shakeel, Nazrul Haq, Wael A. Mahdi, Ibrahim A. Alsarra, Sultan Alshehri, Miteb Alenazi and Abdulrahman Alwhaibi

Materials 2022, 15(22), 8274; https://doi.org/10.3390/ma15228274 - 21 Nov 2022

Cited by 3 | Viewed by 2069

Abstract

The solubilization and thermodynamic analysis of isotretinoin (ITN) in eleven distinct green solvents, such as water, methyl alcohol (MeOH), ethyl alcohol (EtOH), 1-butyl alcohol (1-BuOH), 2-butyl alcohol (2-BuOH), ethane-1,2-diol (EG), propane-1,2-diol (PG), polyethylene glycol-400 (PEG-400), ethyl acetate (EA), Transcutol-HP (THP), and dimethyl sulfoxide (DMSO) was studied at several temperatures and a fixed atmospheric pressure. The equilibrium approach was used to measure the solubility of ITN, and the Apelblat, van’t Hoff, and Buchowski–Ksiazczak λh models were used to correlate the results. The overall uncertainties were less than 5.0% for all the models examined. The highest ITN mole fraction solubility was achieved as 1.01 × 10⁻¹ in DMSO at 318.2 K; however, the least was achieved as 3.16 × 10⁻⁷ in water at 298.2 K. ITN solubility was found to be enhanced with an increase in temperature and the order in which it was soluble in several green solvents at 318.2 K was as follows: DMSO (1.01 × 10⁻¹) > EA (1.73 × 10⁻²) > PEG-400 (1.66 × 10⁻²) > THP (1.59 × 10⁻²) > 2-BuOH (6.32 × 10⁻³) > 1-BuOH (5.88 × 10⁻³) > PG (4.83 × 10⁻³) > EtOH (3.51 × 10⁻³) > EG (3.49 × 10⁻³) > MeOH (2.10 × 10⁻³) > water (1.38 × 10⁻⁶). ITN–DMSO showed the strongest solute–solvent interactions when compared to the other ITN and green solvent combinations. According to thermodynamic studies, ITN dissolution was endothermic and entropy-driven in all of the green solvents tested. The obtained outcomes suggested that DMSO appears to be the best green solvent for ITN solubilization. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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16 pages, 1529 KiB

Open AccessArticle

Solubility and Thermodynamic Properties of Febuxostat in Various (PEG 400 + Water) Mixtures

by Adel F. Alghaith, Wael A. Mahdi, Nazrul Haq, Sultan Alshehri and Faiyaz Shakeel

Materials 2022, 15(20), 7318; https://doi.org/10.3390/ma15207318 - 19 Oct 2022

Cited by 1 | Viewed by 1651

Abstract

The solubility of the poorly soluble medicine febuxostat (FXT) (3) in various {polyethylene glycol 400 (PEG 400) (1) + water (H₂O) (2)} mixtures has been examined at 298.2–318.2 K and 101.1 kPa. FXT solubility was measured using an isothermal method and correlated with “van’t Hoff, Apelblat, Buchowski–Ksiazczak λh, Yalkowsky–Roseman, Jouyban–Acree, and Jouyban–Acree-van’t Hoff models”. FXT mole fraction solubility was enhanced via an increase in temperature and PEG 400 mass fraction in {(PEG 400 (1) + H₂O (2)} mixtures. Neat PEG 400 showed the highest mole fraction solubility of FXT (3.11 × 10^–2 at 318.2 K), while neat H₂O had the lowest (1.91 × 10^–7 at 298.2 K). The overall error value was less than 6.0% for each computational model, indicating good correlations. Based on the positive values of apparent standard enthalpies (46.72–70.30 kJ mol⁻¹) and apparent standard entropies (106.4–118.5 J mol⁻¹ K⁻¹), the dissolution of FXT was “endothermic and entropy-driven” in all {PEG 400 (1) + H₂O (2)} mixtures examined. The main mechanism for FXT solvation in {PEG 400 (1) + H₂O (2)} mixtures was discovered to be an enthalpy-driven process. In comparison to FXT-H₂O, FXT-PEG 400 showed the strongest molecular interactions. In conclusion, these results suggested that PEG 400 has considerable potential for solubilizing a poorly soluble FXT in H₂O. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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12 pages, 3913 KiB

Open AccessArticle

A Green High-Performance Thin-Layer Chromatography Method for the Determination of Caffeine in Commercial Energy Drinks and Formulations

by Ahmed I. Foudah, Faiyaz Shakeel, Mohammad A. Salkini, Sultan Alshehri, Mohammed M. Ghoneim and Prawez Alam

Materials 2022, 15(9), 2965; https://doi.org/10.3390/ma15092965 - 19 Apr 2022

Cited by 10 | Viewed by 2685

Abstract

The literature on green analytical approaches for caffeine estimation is limited. As a consequence, this study aimed to establish a reverse-phase high-performance thin-layer chromatography (HPTLC) technique for caffeine estimation in a variety of commercial energy drinks (ED) and pharmaceutical formulations that is rapid, sensitive, and green. The combination of ethanol-water (55:45 v v⁻¹) was used as a mobile phase. The detection of caffeine was carried out at 275 nm. The green reverse-phase HPTLC method was linear in the concentration range of 50–800 ng band⁻¹. Furthermore, the developed method for caffeine estimation was simple, quick, economical, accurate, precise, robust, sensitive, and green. The amount of caffeine in different marketed ED (ED1–ED10) was recorded in the range of 21.02–37.52 mg 100 mL⁻¹ using the developed HPTLC method. However, the amount of caffeine in different commercial formulations (F1–F3) was estimated as 10.63–20.30 mg 100 mL⁻¹ using the same method. The “analytical GREEnness (AGREE)” scale for the developed analytical method was predicted to be 0.80, utilizing 12 distinct components of green analytical chemistry, indicating the HPTLC approach’s excellent greener profile. Overall, the developed method for estimating caffeine in marketed ED and dosage forms was found to be reliable. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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19 pages, 8579 KiB

Open AccessArticle

Application of the Solute–Solvent Intermolecular Interactions as Indicator of Caffeine Solubility in Aqueous Binary Aprotic and Proton Acceptor Solvents: Measurements and Quantum Chemistry Computations

by Tomasz Jeliński, Maciej Kubsik and Piotr Cysewski

Materials 2022, 15(7), 2472; https://doi.org/10.3390/ma15072472 - 27 Mar 2022

Cited by 12 | Viewed by 4020

Abstract

The solubility of caffeine in aqueous binary mixtures was measured in five aprotic proton acceptor solvents (APAS) including dimethyl sulfoxide, dimethylformamide, 1,4-dioxane, acetonitrile, and acetone. The whole range of concentrations was studied in four temperatures between 25 °C and 40 °C. All systems exhibit a strong cosolvency effect resulting in non-monotonous solubility trends with changes of the mixture composition and showing the highest solubility at unimolar proportions of organic solvent and water. The observed solubility trends were interpreted based on the values of caffeine affinities toward homo- and hetero-molecular pairs formation, determined on an advanced quantum chemistry level including electron correlation and correction for vibrational zero-point energy. It was found that caffeine can act as a donor in pairs formation with all considered aprotic solvents using the hydrogen atom attached to the carbon in the imidazole ring. The computed values of Gibbs free energies of intermolecular pairs formation were further utilized for exploring the possibility of using them as potential solubility prognostics. A semi-quantitative relationship (R² = 0.78) between caffeine affinities and the measured solubility values was found, which was used for screening for new greener solvents. Based on the values of the environmental index (EI), four morpholine analogs were considered and corresponding caffeine affinities were computed. It was found that the same solute–solvent structural motif stabilizes hetero-molecular pairs suggesting their potential applicability as greener replacers of traditional aprotic proton acceptor solvents. This hypothesis was confirmed by additional caffeine solubility measurements in 4-formylmorpholine. This solvent happened to be even more efficient compared to DMSO and the obtained solubility profile follows the cosolvency pattern observed for other aprotic proton acceptor solvents. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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14 pages, 1543 KiB

Open AccessArticle

A Greener Stability-Indicating High-Performance Thin-Layer Chromatography Approach for the Estimation of Topiramate

by Mohammed H. Alqarni, Faiyaz Shakeel, Wael A. Mahdi, Ahmed I. Foudah, Tariq M. Aljarba, Sultan Alshehri, Mohammed M. Ghoneim and Prawez Alam

Materials 2022, 15(5), 1731; https://doi.org/10.3390/ma15051731 - 25 Feb 2022

Cited by 1 | Viewed by 2178

Abstract

Despite various reported analytical methods for topiramate (TPM) analysis, greener analytical approaches are scarce in literature. As a consequence, the objective of the current research is to design a normal-phase stability-indicating high-performance thin-layer chromatography (SI-HPTLC) methodology for TPM analysis in marketed tablet dosage forms that is rapid, sensitive, and greener. TPM was derivatized densitometrically and analyzed at 423 nm in visible mode with anisaldehyde-sulfuric acid as the derivatizing agent. The greener SI-HPTLC technique was linear in the 30–1200 ng band⁻¹ range. In addition, the suggested SI-HPTLC methodology for TPM analysis was simple, rapid, cheaper, precise, robust, sensitive, and environmentally friendly. The greener SI-HPTLC method was able to detect TPM along with its degradation products under acid, base, and oxidative degradation conditions. However, no TPM degradation was recorded under thermal and photolytic stress conditions. TPM contents in commercial tablet dosage forms were recorded as 99.14%. Using 12 different principles of green analytical chemistry, the overall analytical GREEnness (AGREE) score for the greener SI-HPTLC method was calculated to be 0.76, confirming the proposed normal-phase SI-HPTLC method’s good greener nature. Overall, these results demonstrated that the suggested SI-HPTLC technique for TPM measurement in pharmaceutical products was reliable and selective. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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22 pages, 4251 KiB

Open AccessArticle

Experimental and Theoretical Screening for Green Solvents Improving Sulfamethizole Solubility

by Piotr Cysewski, Maciej Przybyłek and Rafal Rozalski

Materials 2021, 14(20), 5915; https://doi.org/10.3390/ma14205915 - 9 Oct 2021

Cited by 20 | Viewed by 3144

Abstract

Solubility enhancement of poorly soluble active pharmaceutical ingredients is of crucial importance for drug development and processing. Extensive experimental screening is limited due to the vast number of potential solvent combinations. Hence, theoretical models can offer valuable hints for guiding experiments aimed at providing solubility data. In this paper, we explore the possibility of applying quantum-chemistry-derived molecular descriptors, adequate for development of an ensemble of neural networks model (ENNM), for solubility computations of sulfamethizole (SMT) in neat and aqueous binary solvent mixtures. The machine learning procedure utilized information encoded in σ-potential profiles computed using the COSMO-RS approach. The resulting nonlinear model is accurate in backcomputing SMT solubility and allowed for extensive screening of green solvents. Since the experimental characteristics of SMT solubility are limited, the data pool was extended by new solubility measurements in water, five neat organic solvents (acetonitrile, N,N-dimethylformamide, dimethyl sulfoxide, 1,4-dioxane, and methanol), and their aqueous binary mixtures at 298.15, 303.15, 308.15, and 313.15 K. Experimentally determined order of decreasing SMT solubility in neat solvents is the following: N,N-dimethylformamide > dimethyl sulfoxide > methanol > acetonitrile > 1,4dioxane >> water, in all studied temperatures. Similar trends are observed for aqueous binary mixtures. Since N,N-dimethylformamide is not considered as a green solvent, the more acceptable replacers were searched for using the developed model. This step led to the conclusion that 4-formylmorpholine is a real alternative to N,N-dimethylformamide, fulfilling all requirements of both high dissolution potential and environmental friendliness. Full article

(This article belongs to the Special Issue Development and Application of Greener Organic Solvents)

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