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Green Analytical Methods for Pharmaceutical, Biomedical, and Environmental Analysis

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

Deadline for manuscript submissions: 30 November 2024 | Viewed by 11291

Special Issue Editors


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Guest Editor
Faculty of Agriculture, Kyushu University, Fukuoka, Japan
Interests: natural medicines; natural cosmetics; natural functional foods; natural aroma; natural dwelling space
Special Issues, Collections and Topics in MDPI journals

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Guest Editor
Pharmaceutical Analytical Chemistry Department, Faculty of Pharmacy, Mansoura University, Mansoura, Egypt
Interests: green analytical chemistry; sample preparation; nanosensors; metabolomics; water analysis; experimental design; chromatography; mass spectrometry

Special Issue Information

Dear Colleagues,

In order to provide sustainable solutions that address real-world issues, the use of analytical methodologies that reduce or eliminate hazardous chemicals to enable faster and more energy-efficient analyses without compromising performance criteria becomes essential. Green analytical techniques are anticipated to open the door for breakthrough techniques and other intriguing new applications in various fields, including pharmaceutical and environmental analysis as well as food authentication. In this instance, analytes such as pharmaceuticals, phytochemical metabolites, contaminants, and others could be determined by green sensing technologies to replace conventional hazardous ones. Areas to be covered may include (but are not limited to) the following:

  • Development and application of green solvents in sample preparation.
  • Development of novel sorbents for SPE and SPME applications.
  • Development of nanomaterial biosensors for the analysis of pharmaceuticals, contaminants, or food components in various matrices.
  • Application of green solvents in chromatographic techniques as mobile-phase additives or stationary-phase modifiers.
  • Improvements in hardware components resulting in the development of portable devices.

We are pleased to invite you to contribute your original research works (full research articles or high-quality reviews) to this Special Issue. We believe that the most recent findings in this area will inspire collaborations between researchers and innovative ideas for the evolution of the green analytical chemistry concept.

Dr. Kuniyoshi Shimizu
Dr. Asmaa Kamal El-Deen
Guest Editors

Manuscript Submission Information

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Keywords

  • green analytical chemistry
  • pharmaceutical
  • contaminants
  • sample preparation
  • green solvents
  • solid-phase microextraction
  • dispersive liquid–liquid microextraction
  • ionic liquids
  • deep eutectic solvents
  • supramolecular solvents
  • nanomaterials
  • carbon dots
  • sensors
  • micellar liquid chromatography

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Published Papers (6 papers)

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Research

21 pages, 2548 KiB  
Article
Green Microfluidic Method for Sustainable and High-Speed Analysis of Basic Amino Acids in Nutritional Supplements
by Iva Pukleš, Csilla Páger, Nikola Sakač, Bojan Šarkanj, Dean Marković, Marija Kraševac Sakač and Marija Jozanović
Molecules 2024, 29(23), 5554; https://doi.org/10.3390/molecules29235554 - 25 Nov 2024
Viewed by 367
Abstract
Amino acids (AAs) have broad nutritional, therapeutic, and medical significance and thus are one of the most common active ingredients of nutritional supplements. Analytical strategies for determining AAs are high-priced and often limited to methods that require modification of AA polarity or incorporation [...] Read more.
Amino acids (AAs) have broad nutritional, therapeutic, and medical significance and thus are one of the most common active ingredients of nutritional supplements. Analytical strategies for determining AAs are high-priced and often limited to methods that require modification of AA polarity or incorporation of an aromatic moiety. The aim of this work was to develop a new method for the determination of L-arginine, L-ornithine, and L-lysine on low-cost microchip electrophoresis instrumentation conjugated with capacitively coupled contactless conductivity detection. A solution consisting of 0.3 M acetic acid and 1 × 10−5 M iminodiacetic acid has been identified as the optimal background electrolyte, ensuring the shortest possible analysis time. The short migration times of amino acids (t ≤ 64 s) and method simplicity resulted in high analysis throughput with high precision and linearity (R2 0.9971). The limit of detection values ranged from 0.15 to 0.19 × 10−6 M. The accuracy of the proposed method was confirmed by recovery measurements. The results were compared with CE-UV-VIS and HPLC-DAD methods and showed good agreement. This work represents the first successful demonstration of the ME-C4D analysis of L-arginine, L-ornithine, and L-lysine in real samples. Full article
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21 pages, 3812 KiB  
Article
Multi-Elemental Analysis of Hair and Fingernails Using Energy-Dispersive X-ray Fluorescence (ED XRF) Method Supported by Inductively Coupled Plasma Mass Spectrometry (ICP MS)
by Zofia Mierzyńska, Maria Niemirska, Kacper Zgonina, Tomasz Bieńkowski, Krzysztof Hryniów, Paweł Świder and Katarzyna Pawlak
Molecules 2024, 29(4), 773; https://doi.org/10.3390/molecules29040773 - 7 Feb 2024
Viewed by 1985
Abstract
This work compared the multi-element analysis of human hair and nails using inductively coupled plasma mass spectrometry (ICP MS) with an easy, fast, cheap, non-destructive method using energy-dispersive x-ray fluorescence (ED XRF). The ICP MS-based method was more sensitive (over 30 elements could [...] Read more.
This work compared the multi-element analysis of human hair and nails using inductively coupled plasma mass spectrometry (ICP MS) with an easy, fast, cheap, non-destructive method using energy-dispersive x-ray fluorescence (ED XRF). The ICP MS-based method was more sensitive (over 30 elements could be quantified) and costly (requiring more time, samples, and chemicals). The EDX-based method required laboratory and certified reference materials made of hair for instrument calibration. It was less sensitive (16 elements could be quantified: S, Si, Ca, Br, Fe, Cu, Cr, Mg, Si, K, Mn, Ni, Zn, Se, Sr, Pb), but it allowed us to replace troublesome grinding with the dissolution of keratin-based material with an alkalic agent (tetramethylammonium hydroxide, TMAH) and the formation of stable-for-days pellets. This method is simple, enables automation, and, due to the modification of wells in the autosampler of the EDX system via the immersion of home-designed inserts, it requires smaller amounts of biological material and binder (down to 70 mg instead of 500 mg required by commercially available instrument) to perform analysis. It was concluded that the EDX-based method offers complementary selectivity and sensitivity to ICP MS with the possibility of sample reuse for further analysis. Full article
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13 pages, 817 KiB  
Article
Simultaneous Determination of Steroids and NSAIDs, Using DLLME-SFO Extraction and HPLC Analysis, in Milk and Eggs Collected from Rural Roma Communities in Transylvania, Romania
by Mihaela Cătălina Herghelegiu, Vlad Alexandru Pănescu, Victor Bocoș-Bințințan, Radu-Tudor Coman, Vidar Berg, Jan Ludvig Lyche, Maria Concetta Bruzzoniti and Mihail Simion Beldean-Galea
Molecules 2024, 29(1), 96; https://doi.org/10.3390/molecules29010096 - 22 Dec 2023
Cited by 2 | Viewed by 1232
Abstract
This research aims to determine five steroids and four non-steroidal anti-inflammatory drugs in milk and egg samples collected from rural Roma communities in Transylvania, Romania. Target compounds were extracted from selected matrices by protein precipitation, followed by extract purification by dispersive liquid–liquid microextraction [...] Read more.
This research aims to determine five steroids and four non-steroidal anti-inflammatory drugs in milk and egg samples collected from rural Roma communities in Transylvania, Romania. Target compounds were extracted from selected matrices by protein precipitation, followed by extract purification by dispersive liquid–liquid microextraction based on solidification of floating organic droplets. The extraction procedure was optimized using a 24 full factorial experimental design. Good enrichment factors (87.64–122.07 milk; 26.97–38.72 eggs), extraction recovery (74.49–103.76% milk; 75.64–108.60% eggs), and clean-up of the sample were obtained. The method detection limits were 0.74–1.77 µg/L for milk and 2.39–6.02 µg/kg for eggs, while the method quantification limits were 2.29–5.46 µg/L for milk and 7.38–18.65 µg/kg for eggs. The steroid concentration in milk samples was <MDL up to 4.30 µg/L, decreasing from 17α-ethinyl estradiol, 17β-estradiol, and estrone to estriol. The NSAID concentration was <MDL up to 3.41 µg/L, decreasing from ibuprofen, diclofenac, and ketoprofen to naproxen. The steroid concentration in the egg samples was <MDL to 2.79 µg/kg, with all steroids detected, while the concentration of NSAIDs was <MDL to 2.28 µg/kg, with only ibuprofen, ketoprofen, and naproxen detected. The developed protocol was successfully applied to the analysis of target compounds in real milk and egg samples. Full article
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16 pages, 2797 KiB  
Article
One-Step Microwell Plate-Based Spectrofluorimetric Assay for Direct Determination of Statins in Bulk Forms and Pharmaceutical Formulations: A Green Eco-Friendly and High-Throughput Analytical Approach
by Ibrahim A. Darwish, Hany W. Darwish, Nourah Z. Alzoman and Awadh M. Ali
Molecules 2023, 28(6), 2808; https://doi.org/10.3390/molecules28062808 - 20 Mar 2023
Cited by 1 | Viewed by 1794
Abstract
This study describes the development of a one-step microwell spectrofluorimetric assay (MW-SFA) with high sensitivity and throughput for the determination of four statins in their pharmaceutical and formulations (tablets). These statins were pitavastatin (PIT), fluvastatin (FLU), rosuvastatin (ROS) and atorvastatin (ATO). The MW-SFA [...] Read more.
This study describes the development of a one-step microwell spectrofluorimetric assay (MW-SFA) with high sensitivity and throughput for the determination of four statins in their pharmaceutical and formulations (tablets). These statins were pitavastatin (PIT), fluvastatin (FLU), rosuvastatin (ROS) and atorvastatin (ATO). The MW-SFA involves the measurement of the native fluorescence of the statin aqueous solutions. The assay was conducted in white opaque 96-microwell plates, and the fluorescence intensities of the solutions were measured by using a fluorescence microplate reader. The optimum conditions of the assay were established; under which, linear relationships with good correlation coefficients (0.9991–0.9996) were found between the fluorescence intensity and the concentration of the statin drug in a range of 0.2–200 µg mL–1 with limits of detection in a range of 0.1–4.1 µg mL–1. The proposed MW-SFA showed high precision, as the values of the relative standard deviations did not exceed 2.5%. The accuracy of the assay was proven by recovery studies, as the recovery values were 99.5–101.4% (±1.4–2.1%). The assay was applied to the determination of the investigated statins in their tablets. The results were statistically compared with those obtained by a reference method and the results proved to have comparable accuracy and precision of both methods, as evidenced by the t- and F-tests, respectively. The green and eco-friendly feature of the proposed assay was assessed by four different metric tools, and all the results proved that the assay meets the requirements of green and eco-friendly analytical approaches. In addition, ever-increasing miniaturization as handling of large numbers of micro-volume samples simultaneously in the proposed assay gave it a high-throughput feature. Therefore, the assay is a valuable tool for the rapid routine application in the pharmaceutical quality control units for the determination of statins. Full article
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14 pages, 2842 KiB  
Article
A Novel Quantum Dots-Based Fluorescent Sensor for Determination of the Anticancer Dacomitinib: Application to Dosage Forms
by Manal A. Alossaimi, Heba Elmansi, Mai Alajaji, Ali Altharawi, Abdulmalik S. A. Altamimi and Galal Magdy
Molecules 2023, 28(5), 2351; https://doi.org/10.3390/molecules28052351 - 3 Mar 2023
Cited by 24 | Viewed by 3051
Abstract
One of the most promising drugs recently approved for the treatment of various types of cancer is dacomitinib, which belongs to the tyrosine kinase inhibitor class. The US Food and Drugs Administration (FDA) has recently approved dacomitinib as a first-line treatment for patients [...] Read more.
One of the most promising drugs recently approved for the treatment of various types of cancer is dacomitinib, which belongs to the tyrosine kinase inhibitor class. The US Food and Drugs Administration (FDA) has recently approved dacomitinib as a first-line treatment for patients suffering from non-small cell lung cancer (NSCLC) with epidermal growth factor receptor (EGFR) mutations. The current study proposes the design of a novel spectrofluorimetric method for determining dacomitinib based on newly synthesized nitrogen-doped carbon quantum dots (N-CQDs) as fluorescent probes. The proposed method is simple and does not require pretreatment or preliminary procedures. Since the studied drug does not have any fluorescent properties, the importance of the current study is magnified. When excited at 325 nm, N-CQDs exhibited native fluorescence at 417 nm, which was quantitatively and selectively quenched by the increasing concentrations of dacomitinib. The developed method involved the simple and green microwave-assisted synthesis of N-CQDs, using orange juice as a carbon source and urea as a nitrogen source. The characterization of the prepared quantum dots was performed using different spectroscopic and microscopic techniques. The synthesized dots had consistently spherical shapes and a narrow size distribution and demonstrated optimal characteristics, including a high stability and a high fluorescence quantum yield (25.3%). When assessing the effectiveness of the proposed method, several optimization factors were considered. The experiments demonstrated highly linear quenching behavior across the concentration range of 1.020.0 μg/mL with a correlation coefficient (r) of 0.999. The recovery percentages were found to be in the range of 98.50–100.83% and the corresponding relative standard deviation (%RSD) was 0.984. The proposed method was shown to be highly sensitive with a limit of detection (LOD) as low as 0.11 μg/mL. The type of mechanism by which quenching took place was also investigated by different means and was found to be static with a complementary inner filter effect. For quality purposes, the assessment of the validation criteria adhered to the ICHQ2(R1) recommendations. Finally, the proposed method was applied to a pharmaceutical dosage form of the drug (Vizimpro® Tablets) and the obtained results were satisfactory. Considering the eco-friendly aspect of the suggested methodology, using natural materials to synthesize N-CQDs and water as a diluting solvent added to its greenness profile. Full article
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19 pages, 3651 KiB  
Article
Prospective of Agro-Waste Husks for Biogenic Synthesis of Polymeric-Based CeO2/NiO Nanocomposite Sensor for Determination of Mebeverine Hydrochloride
by Gamal A. E. Mostafa, Maha F. El-Tohamy and Haitham Alrabiah
Molecules 2023, 28(5), 2095; https://doi.org/10.3390/molecules28052095 - 23 Feb 2023
Cited by 5 | Viewed by 1370
Abstract
Background: The remarkable properties of nickel oxide (NiO) and cerium oxide (CeO2) nanostructures have attracted considerable interest in these nanocomposites as potential electroactive materials for sensor construction. Methods: The mebeverine hydrochloride (MBHCl) content of commercial formulations was determined in this study [...] Read more.
Background: The remarkable properties of nickel oxide (NiO) and cerium oxide (CeO2) nanostructures have attracted considerable interest in these nanocomposites as potential electroactive materials for sensor construction. Methods: The mebeverine hydrochloride (MBHCl) content of commercial formulations was determined in this study using a unique factionalized CeO2/NiO-nanocomposite-coated membrane sensor. Results: Mebeverine-phosphotungstate (MB-PT) was prepared by adding phosphotungstic acid to mebeverine hydrochloride and mixing with a polymeric matrix (polyvinyl chloride, PVC) and plasticizing agent o-nitrophenyl octyl ether. The new suggested sensor showed an excellent linear detection range of the selected analyte at 1.0 × 10−8–1.0 × 10−2 mol L−1 with regression equation EmV = (−29.429 ± 0.2) log [MB] + 347.86. However, the unfunctionalized sensor MB–PT displayed less linearity at 1.0 × 10−5–1.0 × 10−2 mol L−1 drug solution with regression equation EmV = (−26.603 ± 0.5) log [MB] + 256.81. By considering a number of factors, the applicability and validity of the suggested potentiometric system were improved following the rules of analytical methodological requirements. Conclusion: The created potentiometric technique worked well for determining MB in bulk substance and in medical commercial samples. Full article
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