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Advances towards Green Analytical Chemistry

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

Deadline for manuscript submissions: closed (30 September 2020) | Viewed by 33557

Special Issue Editors


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Guest Editor
Laboratorio de Materiales para Análisis Químicos (MAT4LL), Departamento de Química, Unidad Departamental de Química Analítica, Facultad de Ciencias, Universidad de La Laguna, Avda. Astrofísico Francisco Sánchez s/n, 38200 La Laguna, Tenerife, Spain
Interests: microextraction methods; miniaturized analytical sample preparation; ionic liquids and derivatives; metal-organic frameworks; environmental analysis
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Guest Editor
Department of Chemistry (Analytical Chemistry Division), Universidad de la Laguna, Tenerife, Spain
Interests: analytical sample preparation; microextraction; ionic liquids; metal–organic frameworks, polymers; environemntal analysis, bioclinical analysis; food analysis; chromatography

Special Issue Information

Dear Colleagues,

The incorporation of the Green Chemistry requirements within the analytical process has been highly pursued in recent years. In this sense, efforts have shifted towards the development of green analytical sample preparation methods and analytical separation techniques. The proposed strategies to improve the sustainability of analytical protocols are mainly based on the miniaturization and/or automation of the process, the reduction or even elimination of organic solvents and/or toxic reagents required in the procedure, and the design and incorporation of new solvents and sorbents with enhanced environmentally friendly characteristics.
This Special Issue aims to address recent advances in the development of greener tools applied in analytical methodologies, including improvements of the procedures and instrumentation, together with the incorporation of new materials. The use of already proposed sustainable technologies is also covered as long as they are applied for a specific challenging application as an alternative to conventional approaches.
We warmly invite colleagues to contribute to this Special Issue with original research articles or review articles. We believe that this collection will have a significant impact in the analytical research community.

This Special Issue was supported by the Sample Preparation Task Force and Network, supported by the Division of Analytical Chemistry of the European Chemical Society.

Verónica Pino
Idaira Pacheco-Fernández
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

  • Green analytical methods
  • Miniaturization
  • Automation
  • Solvent-free methods
  • Green solvents
  • Ionic liquids
  • Deep eutectic solvents
  • Supramolecular solvents
  • Nanomaterials
  • Biomaterials

Published Papers (7 papers)

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Research

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10 pages, 1183 KiB  
Article
Solubility and Thermal Degradation of Quercetin in CO2-Expanded Liquids
by Larissa P. Cunico, Andrés Medina Cobo, Said Al-Hamimi and Charlotta Turner
Molecules 2020, 25(23), 5582; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25235582 - 27 Nov 2020
Cited by 9 | Viewed by 2182
Abstract
The solubility of quercetin and its thermal degradation was studied in CO2-expanded ethanol and ethyl lactate. An equipment setup was constructed that enabled the separation of the products of degradation while quantifying the solubility of quercetin. Three different conditions of temperature [...] Read more.
The solubility of quercetin and its thermal degradation was studied in CO2-expanded ethanol and ethyl lactate. An equipment setup was constructed that enabled the separation of the products of degradation while quantifying the solubility of quercetin. Three different conditions of temperature were analyzed (308, 323, and 343 K) at 10 MPa. Higher solubility and thermal degradation of quercetin were observed for CO2-expanded ethyl lactate in comparison with CO2-expanded ethanol. At the same time, as the amount of CO2 was increased in the CO2-expanded liquids mixtures, the thermal degradation of quercetin decreased for almost all the conditions of temperature considered in this work. The importance of considering thermal degradation while performing solubility measurements of compounds that are thermally unstable such as quercetin was highlighted. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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17 pages, 3280 KiB  
Article
Evaluation of Structurally Different Ionic Liquid-Based Surfactants in a Green Microwave-Assisted Extraction for the Flavonoids Profile Determination of Mangifera sp. and Passiflora sp. Leaves from Canary Islands
by Kristýna Moučková, Idaira Pacheco-Fernández, Juan H. Ayala, Petra Bajerová and Verónica Pino
Molecules 2020, 25(20), 4734; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25204734 - 15 Oct 2020
Cited by 8 | Viewed by 3359
Abstract
Aqueous solutions of ionic liquids (ILs) with surface active properties were used as extraction solvents, taking advantage of their impressive solvation properties, in a green microwave-assisted solid-liquid extraction method (IL-MA-SLE) for the extraction of flavonoids from passion fruit and mango leaves. The extraction [...] Read more.
Aqueous solutions of ionic liquids (ILs) with surface active properties were used as extraction solvents, taking advantage of their impressive solvation properties, in a green microwave-assisted solid-liquid extraction method (IL-MA-SLE) for the extraction of flavonoids from passion fruit and mango leaves. The extraction method was combined with high-performance liquid chromatography and photodiode-array detection (HPLC-PDA) and optimized by response surface methodology using the Box-Behnken experimental design. Under optimum conditions, the extraction efficiency of six structurally different IL-based surfactants was evaluated. Thus, imidazolium-, guanidinium- and pyridinium-type ILs with different tailorable characteristics, such as side chain length and multicationic core, were assessed. The decylguanidinium chloride ([C10Gu+][Cl]) IL-based surfactant was selected as key material given its superior performance and its low cytotoxicity, for the determination of flavonoids of several samples of Passiflora sp. and Mangifera sp. leaves from the Canary Islands, and using as target analytes: rutin, quercetin and apigenin. The analysis of 50 mg of plant material only required 525 µL of the low cytotoxic IL-based surfactant solution at 930 mM, 10.5 min of microwave irradiation at 30 °C and 50 W, which involves a simpler, faster, more efficient and greener method in comparison with other strategies reported in the literature for obtaining bioactive compounds profiles from plants. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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16 pages, 2905 KiB  
Article
Green Analytical Methods of Antimalarial Artemether-Lumefantrine Analysis for Falsification Detection Using a Low-Cost Handled NIR Spectrometer with DD-SIMCA and Drug Quantification by HPLC
by Moussa Yabré, Ludivine Ferey, Abdoul Karim Sakira, Camille Bonmatin, Clotilde Fauré, Touridomon Issa Somé and Karen Gaudin
Molecules 2020, 25(15), 3397; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25153397 - 27 Jul 2020
Cited by 13 | Viewed by 6611
Abstract
Two green analytical approaches have been developed for the analysis of antimalarial fixed dose tablets of artemether and lumefantrine for quality control. The first approach consisted of investigating the qualitative performance of a low-cost handheld near-infrared spectrometer in combination with the principal component [...] Read more.
Two green analytical approaches have been developed for the analysis of antimalarial fixed dose tablets of artemether and lumefantrine for quality control. The first approach consisted of investigating the qualitative performance of a low-cost handheld near-infrared spectrometer in combination with the principal component analysis as an exploratory tool to identify trends, similarities, and differences between pharmaceutical samples, before applying the data driven soft independent modeling of class analogy (DD-SIMCA) as a one-class classifier for proper drug falsification detection with 100% of both sensitivity and specificity in the studied cases. Despite its limited spectral range and low resolution, the handheld device allowed detecting falsified drugs with no active pharmaceutical ingredient and identifying specifically a pharmaceutical tablet brand name. The second approach was the quantitative analysis based on the green and fast RP-HPLC technique using ethanol as a green organic solvent and acetic acid as a green pH modifier. The optimal separation was achieved in 7 min using a mobile phase composed of ethanol 96% and 10 mM of acetic acid pH 3.35 (63:37, v/v). The developed method was validated according to the total error approach based on an accuracy profile, was applied to the analysis of tablets, and allowed confirming falsified drugs detected by spectroscopy. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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11 pages, 689 KiB  
Article
A New Method for Determination of Thymol and Carvacrol in Thymi herba by Ultraperformance Convergence Chromatography (UPC2)
by Xiaoqiang Chang, Peng Sun, Yue Ma, Dongchen Han, Yifan Zhao, Yue Bai, Dong Zhang and Lan Yang
Molecules 2020, 25(3), 502; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25030502 - 23 Jan 2020
Cited by 13 | Viewed by 4670
Abstract
Ultraperformance convergence chromatography is an environmentally friendly analytical technique for dramatically reducing the use of organic solvents compared to conventional chromatographic methods. In this study, a rapid and sensitive ultraperformance convergence chromatography method was firstly established for quantification of thymol and carvacrol, two [...] Read more.
Ultraperformance convergence chromatography is an environmentally friendly analytical technique for dramatically reducing the use of organic solvents compared to conventional chromatographic methods. In this study, a rapid and sensitive ultraperformance convergence chromatography method was firstly established for quantification of thymol and carvacrol, two positional isomers of a major bioactive in the volatile oil of Thymi herba, the dried leaves and flowers of Thymus mongolicus or Thymus przewalskii, known in China as “Dijiao.” Using a TrefoilTM CEL1 column, thymol and carvacrol were separated in less than 2.5 min and resolution was enhanced. The method was validated with respect to precision, accuracy, and linearity according to the National Medical Products Administration guidelines. The optimized method exhibited good linear correlation (r = 0.9998−0.9999), excellent precision (relative standard deviations (RSDs) < 1.50%), and acceptable recoveries (87.29–102.89%). The limits of detection for thymol and carvacrol were 1.31 and 1.57 ng/L, respectively, while their corresponding limits of quantification were 2.63 and 3.14 ng/L. Finally, the quantities of the two compounds present in 16 T. mongolicus and four T. przewalskii samples were successfully evaluated by employing the developed method. It is hoped that the results of this study will serve as a guideline for the quality control of Thymi herba. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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Review

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20 pages, 2402 KiB  
Review
Effervescence-Assisted Microextraction—One Decade of Developments
by Guillermo Lasarte-Aragonés, Rafael Lucena and Soledad Cárdenas
Molecules 2020, 25(24), 6053; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25246053 - 21 Dec 2020
Cited by 23 | Viewed by 3800
Abstract
Dispersive microextraction techniques are key in the analytical sample treatment context as they combine a favored thermodynamics and kinetics isolation of the target analytes from the sample matrix. The dispersion of the extractant in the form of tiny particles or drops, depending on [...] Read more.
Dispersive microextraction techniques are key in the analytical sample treatment context as they combine a favored thermodynamics and kinetics isolation of the target analytes from the sample matrix. The dispersion of the extractant in the form of tiny particles or drops, depending on the technique, into the sample enlarges the contact surface area between phases, thus enhancing the mass transference. This dispersion can be achieved by applying external energy sources, the use of chemicals, or the combination of both strategies. Effervescence-assisted microextraction emerged in 2011 as a new alternative in this context. The technique uses in situ-generated carbon dioxide as the disperser, and it has been successfully applied in the solid-phase and liquid-phase microextraction fields. This minireview explains the main fundamentals of the technique, its potential and the main developments reported. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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13 pages, 3706 KiB  
Review
Implementing Green Analytical Methodologies Using Solid-Phase Microextraction: A Review
by Kayla M. Billiard, Amanda R. Dershem and Emanuela Gionfriddo
Molecules 2020, 25(22), 5297; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25225297 - 13 Nov 2020
Cited by 52 | Viewed by 4299
Abstract
Implementing green analytical methodologies has been one of the main objectives of the analytical chemistry community for the past two decades. Sample preparation and extraction procedures are two parts of analytical method development that can be best adapted to meet the principles of [...] Read more.
Implementing green analytical methodologies has been one of the main objectives of the analytical chemistry community for the past two decades. Sample preparation and extraction procedures are two parts of analytical method development that can be best adapted to meet the principles of green analytical chemistry. The goal of transitioning to green analytical chemistry is to establish new methods that perform comparably—or superiorly—to traditional methods. The use of assessment tools to provide an objective and concise evaluation of the analytical methods’ adherence to the principles of green analytical chemistry is critical to achieving this goal. In this review, we describe various sample preparation and extraction methods that can be used to increase the greenness of a given analytical method. We gave special emphasis to modern microextraction technologies and their important contributions to the development of new green analytical methods. Several manuscripts in which the greenness of a solid-phase microextraction (SPME) technique was compared to other sample preparation strategies using the Green Analytical Procedure Index (GAPI), a green assessment tool, were reviewed. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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22 pages, 12177 KiB  
Review
Magnetic Solid-Phase Extraction of Organic Compounds Based on Graphene Oxide Nanocomposites
by Natalia Manousi, Erwin Rosenberg, Eleni Deliyanni, George A. Zachariadis and Victoria Samanidou
Molecules 2020, 25(5), 1148; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25051148 - 4 Mar 2020
Cited by 53 | Viewed by 7662
Abstract
Graphene oxide (GO) is a chemical compound with a form similar to graphene that consists of one-atom-thick two-dimensional layers of sp2-bonded carbon. Graphene oxide exhibits high hydrophilicity and dispersibility. Thus, it is difficult to be separated from aqueous solutions. Therefore, functionalization [...] Read more.
Graphene oxide (GO) is a chemical compound with a form similar to graphene that consists of one-atom-thick two-dimensional layers of sp2-bonded carbon. Graphene oxide exhibits high hydrophilicity and dispersibility. Thus, it is difficult to be separated from aqueous solutions. Therefore, functionalization with magnetic nanoparticles is performed in order to prepare a magnetic GO nanocomposite that combines the sufficient adsorption capacity of graphene oxide and the convenience of magnetic separation. Moreover, the magnetic material can be further functionalized with different groups to prevent aggregation and extends its potential application. Until today, a plethora of magnetic GO hybrid materials have been synthesized and successfully employed for the magnetic solid-phase extraction of organic compounds from environmental, agricultural, biological, and food samples. The developed GO nanocomposites exhibit satisfactory stability in aqueous solutions, as well as sufficient surface area. Thus, they are considered as an alternative to conventional sorbents by enriching the analytical toolbox for the analysis of trace organic compounds. Full article
(This article belongs to the Special Issue Advances towards Green Analytical Chemistry)
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