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Green Extraction of Natural Products (GENP 2022)

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A special issue of Antioxidants (ISSN 2076-3921). This special issue belongs to the section "Extraction and Industrial Applications of Antioxidants".

Deadline for manuscript submissions: closed (1 October 2023) | Viewed by 26247

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Special Issue Editors

Dr. Marija Badanjak Sabolović

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Faculty of Food Technology and Biotechnology, University of Zagreb, Zagreb, Croatia
Interests: innovative food processing techniques; bioactive compound extraction; antioxidant activity; novel food

Dr. Jana Šic Žlabur

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Guest Editor

Faculty of Agriculture, University of Zagreb, Svetošimunska Cesta 25, 10000 Zagreb, Croatia
Interests: bioactive compounds; phytochemicals; antioxidant properties; green extraction methods; by-products recovery
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Prof. Dr. Mladen Brnčić

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Faculty of Food Technology and Biotechnology, University of Zagreb, Zagreb, Croatia
Interests: bioactive compounds; food preservation high-pressure processing; ultrasound; microwaves; waste and by-products processing and valorization; extraction of bioactive compounds; drying

Prof. Dr. Francisco J. Barba

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Nutrition and Food Science Area, Preventive Medicine and Public Health, Food Science, Toxicology and Forensic Medicine Department, Faculty of Pharmacy, Universitat de València, Avda. Vicent Andrés Estellés, s/n, 46100 Burjassot, Valencia, Spain
Interests: nutrients; bioactive compounds; food preservation; thermal treatment; innovative processing; high-pressure processing; compressed fluids; pulsed electric fields; ultrasound; microwaves; phytochemical purification; phytochemical analysis; compound isolation; bioaccessibility; bioavailability
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Special Issue Information

Dear Colleagues,

The critical focus of the European Green New Deal is to transform existing systems into a modern, resource-efficient, and competitive system with multiple strategies aimed at making our food systems fairer, healthier, and more environmentally friendly. Thus, the main goal should be to develop practices and strategies that make our food systems more sustainable and resilient to various causes of crises (climate, health, etc.) in order to build a food chain that works for consumers, producers, the climate, and the environment. In light of this, the International Congress on Green Extraction of Natural Products (GENP2022) will focus on the valorization of agricultural and food waste, bioprocess resources and innovative conversion technologies, perfume, cosmetics, pharmaceuticals, food, biofuels, chemicals and energy sectors, and the green chemistry market. An overview of advances in green extraction and sustainable processes will be a hot research topic. The entire value chain will be considered, from cultivation, extraction, processing, and recycling to applications: agrofood, nutraceuticals, perfume, cosmetics, chemicals, fuel, and energy. Based on the above, this Special Issue of Antioxidants will cover current research topics and welcomes research contributions that address these issues:

Alternative solvents for green extraction;
Sustainable and clean extraction technologies;
Innovative extraction process design;
Valorization of by-products and biorefinery.

30% Discount to Paper Publishing in the Special Issue Conference attendants who publish papers in Special Issue: "Green Extraction of Natural Products (GENP 2022)"

Dr. Marija Badanjak Sabolović
Dr. Jana Šic Žlabur
Prof. Dr. Mladen Brnčić
Prof. Dr. Francisco J. Barba
Guest Editors

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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. Antioxidants is an international peer-reviewed open access monthly journal published by MDPI.

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Keywords

green extraction methods
valorization and recovery of by-products
possibilities of green recovery of bioactive compounds
innovative and sustainable food processing methods

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Published Papers (10 papers)

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13 pages, 1381 KiB

Open AccessArticle

Scanning Electron Microscopy and Triple TOF-LC-MS-MS Analysis of Polyphenols from PEF-Treated Edible Mushrooms (L. edodes, A. brunnescens, and P. ostreatus)

by Mara Calleja-Gómez, Patricia Roig, Suzana Rimac Brnčić, Francisco J. Barba and Juan Manuel Castagnini

Antioxidants 2023, 12(12), 2080; https://doi.org/10.3390/antiox12122080 - 6 Dec 2023

Cited by 2 | Viewed by 1403

Abstract

Pulsed electric fields (PEF) technology has been used as a sustainable method for extracting antioxidant bioactive compounds from different food matrices. In the present study, the optimal conditions of PEF extraction for mushrooms (2.5 kV/cm, 50 kJ/kg, 6 h) were applied to Lentinula edodes, Agaricus brunnescens, and Pleurotus ostreatus to evaluate the total antioxidant capacity of the extracts, followed by the Triple TOF-LC-MS-MS analysis of the phenolic profile compared to A. bisporus by high-performance liquid chromatography coupled to mass spectrophotometry. In addition, the microporation effect of the technology on the mushroom surface was evaluated using scanning electron microscopy. A comparison was made with a maceration extraction (aqueous stirring for 6 h). The results showed that PEF-assisted extraction enhanced the recovery of antioxidant compounds such as 3,5-dicaffeoylquinic and cinnamic acid with contents up to 236.85 µg/100 g dry weight and 2043.26 µg/100 g dry weight from A. bisporus, respectively. However, mixed results were obtained for certain phenolic compounds, including vanillic acid from L. edodes, ellagic acid from P. ostreatus, and thymol from all mushrooms. These results indicate that the application of PEF technology is effective for the extraction of antioxidant compounds in fungal matrices by creating micropores in cell membranes that allow great recovery in matrices with high content of bioactive compounds. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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28 pages, 4688 KiB

Open AccessArticle

Unlocking the Bioactive Potential of Pomegranate Peels: A Green Extraction Approach

by Giorgio Grillo, Giorgio Capaldi, Kristina Radošević, Željko Jakopović, Ksenija Markov, Mladen Brncic, Lorenzo Gallina, Emanuela Calcio Gaudino and Giancarlo Cravotto

Antioxidants 2023, 12(10), 1796; https://doi.org/10.3390/antiox12101796 - 23 Sep 2023

Cited by 3 | Viewed by 2369

Abstract

Pomegranate (Punica granatum L.) is well known for its high content of bioactives, including polyphenols, flavonoids, and tannins, which have been shown to exhibit a wide range of biological activities, such as antioxidant, antimicrobial, and anticancer effects. It is worth noting that the majority of these molecules are found in the peels, which are usually disposed of after processing, causing a significant amount of waste, amounting to more than 3.6 million t/y. This work investigates microwave-assisted extraction (MAE) in water for the recovery of antioxidants from pomegranate peels (PP), including the optimisation of temperature and extraction times. The total phenolic, anthocyanin, flavonoid, and tannin contents of the recovered extracts were determined, as well as their antioxidant activities, which were found to be 356.35 mgGAE/gExtr, 303.97 µgCy3G/gExtr, 37.28 mgQE/gExtr, 56.48 mgGAE/gExtr, and 5.72 mmolTE/gExtr, respectively (according to the adopted reference). All results were compared with those obtained using a conventional protocol. In addition, the potential for water recycling by means of downstream nanofiltration in optimised MAE was investigated, leading to overall water reuse of approx. 75%. Power consumption (20.92 W/mgGAE) and common green metrics, Reaction Mass Efficiency (RME), E-Factor, and the Process Mass Intensiti/efficiency (PMI, PME), were considered in evaluating the proposed PP valorisation strategy. Finally, the biological activities of the main products were assessed. The antimicrobial properties of the PP extracts against three Gram-positive and three Gram-negative bacteria and their antiproliferative activity towards human cancer cells were tested. S. aureus bacteria was the most susceptible to the PP extracts. All tested products displayed antiproliferative activity against HeLa cells when higher concentrations were tested, with D-PP/NF (obtained from dried PP and sequential nanofiltration) being the most effective. This result was also confirmed via clonogenic analysis, which generally indicated the possible anti-cancer activity of pomegranate peel extracts obtained using this green approach. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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25 pages, 1339 KiB

Open AccessArticle

Optimized Single-Step Recovery of Lipophilic and Hydrophilic Compounds from Raspberry, Strawberry and Blackberry Pomaces Using a Simultaneous Ultrasound-Enzyme-Assisted Extraction (UEAE)

by Morag Davidson, François Louvet, Emmanuelle Meudec, Cornelia Landolt, Karine Grenier, Sandrine Périno, Tan-Sothéa Ouk and Naïma Saad

Antioxidants 2023, 12(10), 1793; https://doi.org/10.3390/antiox12101793 - 22 Sep 2023

Cited by 4 | Viewed by 1387

Abstract

An ultrasound-enzyme-assisted extraction (UEAE) was optimized to extract, simultaneously, the hydrophilic and lipophilic compounds from three berry pomaces (raspberry, strawberry and blackberry). First, an enzyme screening designated a thermostable alkaline protease as the most suitable enzyme to recover, in an aqueous medium, the highest yields of polyphenols and oil in the most efficient way. Secondly, the selected enzyme was coupled to ultrasounds (US) in sequential and simultaneous combinations. The simultaneous US–alkaline enzyme combination was selected as a one-single-step process and was then optimized by definitive screening design (DSD). The optimized parameters were: US amplitude, 20% (raspberry pomace) or 70% (strawberry and blackberry pomaces); pH, 8; E/S ratio, 1% (w/w); S/L ratio, 6% (w/v); extraction time, 30 min; temperature, 60 °C. Compared to conventional extractions using organic solvents, the UEAE extracted all the polyphenols, with around 75% of the active polyphenols (measured by the DPPH^● method) and up to 75% of the initial oil from the berry pomaces. Characterized lipophilic compounds were rich in polyunsaturated fatty acids (PUFAs), tocols and phytosterols. The polyphenolics were analyzed by UPLC-MS/MS; characteristic ellagitannins of the Rosaceae family (sanguiin H-6 or agrimoniin, sanguiin H-10, …) and ellagic acid conjugates were found as the major components. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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13 pages, 2602 KiB

Open AccessArticle

Response Surface Methodology for the Optimization of Flavan-3-ols Extraction from Avocado By-Products via Sonotrode Ultrasound-Assisted Extraction

by María del Carmen Razola-Díaz, Vito Verardo, Eduardo Jesús Guerra-Hernández, Belén García-Villanova Ruiz and Ana María Gómez-Caravaca

Antioxidants 2023, 12(7), 1409; https://doi.org/10.3390/antiox12071409 - 11 Jul 2023

Cited by 4 | Viewed by 1486

Abstract

Avocado peel and seed are the main by-products of avocado processing and are considered as promising sources of phenolic compounds with biological activities. Thus, this research focuses on the establishment, for the first time, of ultrasound-assisted extraction of flavan-3-ols with high antioxidant activity from avocado peel and seed using a sonotrode. Indeed, 2 Box–Behnken designs were performed for 15 experiments, with each design having three independent factors (ratio ethanol/water (v/v), time (min) and amplitude (%)). In both models, the responses included total procyanidins (flavan-3-ols) measured via HPLC-FLD and antioxidant activity measured via DPPH, ABTS and FRAP. The results showed that applying the sonotrode extraction method could increase flavan-3-ols recovery by 54% and antioxidant activity by 62–76% compared to ultrasound bath technology. Therefore, this technology was demonstrated to be a non-thermal, low time-consuming and scalable method that allowed the recovery of flavan-3-ols from avocado by-products that could be used as functional ingredients. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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11 pages, 1973 KiB

Open AccessArticle

Optimization of Conditions for Microwave-Assisted Extraction of Polyphenols from Olive Pomace of Žutica Variety: Waste Valorization Approach

by Ana Marđokić, Angela Estefanía Maldonado, Katalin Klosz, Máté András Molnár, Gyula Vatai and Szilvia Bánvölgyi

Antioxidants 2023, 12(6), 1175; https://doi.org/10.3390/antiox12061175 - 29 May 2023

Cited by 5 | Viewed by 2060

Abstract

Olive pomace is a by-product of olive oil production that is toxic to the environment. The purpose of this study was to evaluate the methods of olive pomace valorization through the implementation of novel technology, the so-called microwave-assisted extraction process. To determine the total polyphenol content (TPC) and antioxidant activity (AA), polyphenol extraction using MAE was performed. Response surface methodology was used to determine the best extraction conditions, whereby the effects of three factors, solid ratio (g/50 mL), time (s), and power (W), were measured. The ferric reducing antioxidant power (FRAP) method was used to assess AA, whereas the spectrophotometric Folin–Ciocalteu (FC) method was used to determine TPC. The highest TPC of 15.30 mg of gallic acid equivalents per gram of dried weight (mg GAE/gdw) was generated after 105 s at 450 W, with a solid concentration of 1 g/50 mL, while the maximum AA was 10 mg of ascorbic acid equivalents per gram of dried weight (mg AAE/gdw). Numerical optimization revealed that 800 W, 180 s, and 1 g/50 mL were the best conditions for obtaining maximum TPC and AA. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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25 pages, 5866 KiB

Open AccessArticle

Exploring the Potential of Supercritical Fluid Extraction of Matricaria chamomilla White Ray Florets as a Source of Bioactive (Cosmetic) Ingredients

by Laura Pastare, Marta Berga, Liene Kienkas, Martins Boroduskis, Anna Ramata-Stunda, Dace Reihmane, Maris Senkovs, Gundars Skudrins and Ilva Nakurte

Antioxidants 2023, 12(5), 1092; https://doi.org/10.3390/antiox12051092 - 12 May 2023

Cited by 5 | Viewed by 2842

Abstract

Aromatic and medicinal plants are a great source of useful bioactive compounds for use in cosmetics, drugs, and dietary supplements. This study investigated the potential of using supercritical fluid extracts obtained from Matricaria chamomilla white ray florets, a kind of industrial herbal byproduct, as a source of bioactive cosmetic ingredients. Response surface methodology to optimize the supercritical fluid extraction process by analyzing the impact of pressure and temperature on yield and the main bioactive compound groups were used. High-throughput 96-well plate spectrophotometric methods were used to analyze the extracts for total phenols, flavonoids, tannins, and sugars, as well as their antioxidant capacity. Gas chromatography and liquid chromatography–mass spectrometry was used to determine the phytochemical composition of the extracts. The extracts were also analyzed for antimicrobial activity, cytotoxicity, phototoxicity, and melanin content. Statistical analysis was performed to establish correlations between the extracts and develop models to predict the targeted phytochemical recovery and chemical and biological activities. The results show that the extracts contained a diverse range of phytochemical classes and had cytotoxic, proliferation-reducing, and antimicrobial activities, making them potentially useful in cosmetic formulations. This study provides valuable insights for further research on the uses and mechanisms of action of these extracts. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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17 pages, 2152 KiB

Open AccessArticle

Ultrasound-Assisted Extraction of Isoquercetin from Ephedra alata (Decne): Optimization Using Response Surface Methodology and In Vitro Bioactivities

by Ezzouhra El Maaiden, Nagib Qarah, Amine Ezzariai, Adil Mazar, Boubker Nasser, Khadija Moustaid, Hassan Boukcim, Abdelaziz Hirich, Lamfeddal Kouisni and Youssef El Kharrassi

Antioxidants 2023, 12(3), 725; https://doi.org/10.3390/antiox12030725 - 15 Mar 2023

Cited by 9 | Viewed by 2705

Abstract

Isoquercetin (ISQ) is reported to be a powerful antioxidant with extremely high bioavailability and structural stability compared to aglycone quercetin. Despite this, it is not well studied due to the limited methods for its extraction. With the growing interest in the research and analysis of ISQ-rich herbs, there is a need to optimize an efficient and rapid method for their extraction. In the present study, the ultrasound-assisted extraction of ISQ from Ephedra alata Decne was optimized by a response surface methodology (RSM) using high-performance liquid chromatography as a separation method. The best possible ranges for extraction time (10–30 min), temperature (50–70 °C), ultrasonic power (60–90 W), solvent-to-solid ratio (50–70 mL/g), and ethanol concentration (50–70%) were determined using a single factor analysis. Subsequently, an optimization of the extraction conditions was performed with RSM using the Box–Behnken design. An ultrasonication time of 10 min, a temperature of 60 °C, a power of 75 W, a solvent-to-solid ratio of 60 mL/g, and an ethanol concentration of 70% were determined to be the optimal conditions for the highest recovery of isoquercetin (1033.96 ± 3.28 µg/g). Furthermore, E. alata powder morphology (using a scanning electron microscope), antioxidant activities, and the inhibition potential of key enzymes involved in skin aging (elastase and collagenase), hyperpigmentation (tyrosinase), diabetes (α-amylase), inflammation (hyaluronidase), and neurodegenerative disorders (cholinesterase) were determined and compared with those using the Soxhlet method. This study established a highly efficient method for ISQ extraction and suggested several potential applications of ISQ in the pharmaceutical and cosmetics industries. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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19 pages, 1588 KiB

Open AccessArticle

Optimization of Ursolic Acid Extraction in Oil from Annurca Apple to Obtain Oleolytes with Potential Cosmeceutical Application

by Maria Maisto, Vincenzo Piccolo, Ettore Novellino, Elisabetta Schiano, Fortuna Iannuzzo, Roberto Ciampaglia, Vincenzo Summa and Gian Carlo Tenore

Antioxidants 2023, 12(2), 224; https://doi.org/10.3390/antiox12020224 - 18 Jan 2023

Cited by 13 | Viewed by 3061

Abstract

Ursolic acid (UA) is a plant-derived molecule with relevant anti-aging activity, which makes this molecule a potential functional active ingredient in cosmetic formulations. The main objectives of this study were to optimize the UA extraction process from Annurca apple (AA) with sunflower oil as a lyophilic food-grade solvent using Response Surface Methodology (RSM) to determine the potential cosmetic application of the obtained extract. The results of RSM analysis showed a maximum UA yield of 784.40 ± 7.579 (μg/mL) obtained under the following optimized conditions: sunflower oil as extraction solvent, 68.85 °C as extraction temperature, and 63 h as extraction time. The HPLC-DAD-HESI-MS/MS analysis performed on the extract obtained under these conditions, named Optimized Annurca Apple Oleolyte (OAAO), led to the identification of twenty-three phenolic and terpenoid molecules and the quantification of eight of them. To explore the biological properties of OAAO, the in vitro antioxidant activity was evaluated by DPPH, ABTS, and FRAP assays, resulting in 16.63 ± 0.22, 5.90 ± 0.49, and 21.72 ± 0.68 μmol Trolox equivalent/g extract, respectively. Moreover, the permeation study has shown that OAAO may be considered a safe and functional ingredient in potential cosmetic formulations. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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15 pages, 2046 KiB

Open AccessArticle

Chemical Compositions, Extraction Optimizations, and In Vitro Bioactivities of Flavonoids from Perilla Leaves (Perillae folium) by Microwave-Assisted Natural Deep Eutectic Solvents

by Xianchao Shang, Manman Zhang, Jing Hu, Yuqin Zhang, Long Yang and Xin Hou

Antioxidants 2023, 12(1), 104; https://doi.org/10.3390/antiox12010104 - 31 Dec 2022

Cited by 16 | Viewed by 3278

Abstract

Natural deep eutectic solvents (NADESs) have been gradually applied to green extraction of active ingredients. In this study, microwave-assisted NADESs were applied to the extraction of flavonoid compounds from perilla leaves. Through comparative experiments, NADES-3 (choline chloride and malic acid at a molar ratio of 1:1) was found to have the highest extraction efficiency of total flavonoids, including apigenin 7-O-caffeoylglucoside, scutellarein 7-O-diglucuronide, luteolin 7-O-diglucuronide, and scutellarein 7-O-glucuronide by HPLC-MS. The following optimal extraction parameters were obtained based on response surface design: water content in NADES of 23%, extraction power of 410 W, extraction time of 31 min, and solid–liquid ratio of 75 mg/mL, leading to the extraction yield of total flavonoids of 72.54 mg/g. Additionally, the strong antimicrobial and antiallergic activity, inhibition of nitrosation, and antioxidant activity of total flavonoids by using NADESs were confirmed. This new extraction method provides a reference for the further exploration of NADES systems and may be widely used for the green extraction of natural active ingredients. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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26 pages, 1013 KiB

Open AccessReview

Sustainable Green Extraction of Carotenoid Pigments: Innovative Technologies and Bio-Based Solvents

by Ángeles Morón-Ortiz, Paula Mapelli-Brahm and Antonio J. Meléndez-Martínez

Antioxidants 2024, 13(2), 239; https://doi.org/10.3390/antiox13020239 - 15 Feb 2024

Cited by 6 | Viewed by 3397

Abstract

Carotenoids are ubiquitous and versatile isoprenoid compounds. The intake of foods rich in these pigments is often associated with health benefits, attributable to the provitamin A activity of some of them and different mechanisms. The importance of carotenoids and their derivatives for the production of foods and health-promotion through the diet is beyond doubt. In the new circular economy paradigm, the recovery of carotenoids in the biorefinery process is highly desirable, for which greener processes and solvents are being advocated for, considering the many studies being conducted at the laboratory scale. This review summarizes information on different extraction technologies (ultrasound, microwaves, pulsed electric fields, pressurized liquid extraction, sub- and supercritical fluid extraction, and enzyme-assisted extraction) and green solvents (ethyl lactate, 2-methyltetrahydrofuran, natural deep eutectic solvents, and ionic liquids), which are potential substitutes for more toxic and less environmentally friendly solvents. Additionally, it discusses the results of the latest studies on the sustainable green extraction of carotenoids. The conclusions drawn from the review indicate that while laboratory results are often promising, the scalability to real industrial scenarios poses a significant challenge. Furthermore, incorporating life cycle assessment analyses is crucial for a comprehensive evaluation of the sustainability of innovative extraction processes compared to industry-standard methods. Full article

(This article belongs to the Special Issue Green Extraction of Natural Products (GENP 2022))

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