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Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches

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A special issue of Plants (ISSN 2223-7747). This special issue belongs to the section "Phytochemistry".

Deadline for manuscript submissions: 31 March 2025 | Viewed by 10560

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Special Issue Editors

Prof. Dr. Grasiele Scaramal Madrona

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Department of Food Engineering, Universidade Estadual de Maringa, Maringa, Brazil
Interests: extraction; characterization and application of bioactive compounds in foods

Dr. Adriano Costa de Camargo

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Nutrition and Food Technology Institute, University of Chile, Santiago 7830490, Chile
Interests: plants
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Prof. Dr. Rúbia Carvalho Gomes Corrêa

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Cesumar Institute of Science, Technology and Innovation-ICETI, Cesumar University–UniCesumar, 1610 Guerdner Venue, Acclimation Gardner, Maringa, Parana, Brazil
Interests: food science and nutrition; sustainable food systems; adding value to agro-industrial waste; production of bioactive compounds; upcycling of food wastes; novel plant-based materials
Special Issues, Collections and Topics in MDPI journals

Dr. Carlos Eduardo Eduardo Barão

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Federal Institute of Parana, Paranavai Campus, Av. Jose Felipe Tequinha, 1400, Paranavai 87703-536, PR, Brazil
Interests: extraction; food science and technology; natural products

Dr. Miria Hespanhol Miranda Reis

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Faculdade de Engenharia Química, Universidade Federal de Uberlândia, Uberlandia, Brazil
Interests: development of fermentative, enzymatic processes, with membranes and environmental technologies

Special Issue Information

Dear Colleagues,

Green chemistry has emerged due to the importance of the use of processes that are environmentally friendly. For extracting natural products, greener and more sustainable alternatives to traditional methods have been explored over the last decade. The knowledge generated by this topic can help society change its habits and behaviors, showing us how certain products and attitudes pose more risks to nature than others. This knowledge also ties into Sustainable Development Goals 2; 11; and, more specifically, 12, which deal with sustainable production and consumption. In this sense, with the aim of providing a new and novel knowledge base via green chemistry for natural products, we would like to invite researchers to participate in this Special Issue. Therefore, this Special Issue will focus on approaches to improve and accelerate extraction efficiency and reduce solvent consumption, such as solvent-based techniques, deep euteric solvents (DES), ultrasound-assisted extraction and microwave-assisted extraction, as well as supercritical fluid extraction and pressurized solvent extraction. However, other related research is highly encouraged. Authors are cordially invited to contribute original research articles as well as review articles. All research will be published as Open Access.

Prof. Dr. Grasiele Scaramal Madrona
Dr. Adriano Costa de Camargo
Prof. Dr. Rubia Carvalho Gomes Correa
Dr. Carlos Eduardo Eduardo Barão
Dr. Miria Hespanhol Miranda Reis
Guest Editors

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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. Plants 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

sustainable extraction
agro-industrial by-products extraction
green extraction
clean technologies
natural ingredients
food security
sustainable development

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Published Papers (10 papers)

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Research

17 pages, 2459 KiB

Open AccessArticle

Optimization of Two Methods for the Rapid and Effective Extraction of Quinine from Cinchona officinalis

by Gianella Ochoa, Leonardo Armijos, Jorge G. Figueroa, Ximena Jaramillo-Fierro and Natalí Solano-Cueva

Plants 2025, 14(3), 364; https://doi.org/10.3390/plants14030364 - 25 Jan 2025

Viewed by 331

Abstract

This study successfully optimized two advanced extraction methods, microwave-assisted extraction (MAE) and ultrasound-assisted extraction (UAE), for the efficient and rapid recovery of quinine from Cinchona officinalis. Among the evaluated parts of the plant, the bark consistently yielded the highest quinine concentration, highlighting its significance as the primary source for alkaloid extraction. The optimized conditions for MAE (65% ethanol, 130 °C, 34 min) achieved a maximum yield of 3.93 ± 0.11 mg/g, while UAE (61% ethanol, 25 °C, 15 min) provided a faster but slightly lower yield of 2.81 ± 0.04 mg/g. These findings confirm the superiority of MAE and UAE over conventional methods like Soxhlet extraction in terms of time efficiency and sustainability. The quantification of quinine using high-performance liquid chromatography (HPLC) coupled with advanced detection methods further validated the reliability and reproducibility of the results. While this study focused on optimizing extraction and quantification parameters, it sets the groundwork for future research into the sustainable utilization and potential valorization of C. officinalis byproducts. These findings not only provide a standardized protocol for extracting quinine but also contribute to the broader application of green chemistry principles in pharmaceutical production. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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14 pages, 284 KiB

Open AccessArticle

Application of the Biorefinery Concept in the Processing of Crambe (Crambe abyssinica Hochst) Seed Defatted Meal in a Pressurized Medium

by Camila da Silva, Jefferson Alessandro Schmitz, Jr., Djéssica Tatiane Raspe, Natália Stevanato, Jaqueline Hoscheid, Marcelino Luiz Gimenes, Beatriz Cervejeira Bolanho Barros and Lúcio Cardozo-Filho

Plants 2025, 14(3), 326; https://doi.org/10.3390/plants14030326 - 22 Jan 2025

Viewed by 607

Abstract

The valorization of byproducts such as defatted meal (DM) is essential for the implementation of a biorefinery structure and can be achieved through the application of emerging technologies, such as pressurized liquid extraction. This work aimed to apply pressurized liquid extraction to obtain products derived from the DM of crambe (Crambe abyssinica Hochst) seeds. The experiments investigated the effect of ethanol percentage in the hydroalcoholic solvent (25%, 50% and 75%, v/v) on the mass extract yield (MEY) and on the composition of the products obtained: phytochemical extract (PE) and processed flour (PF). The PE obtained using 25% ethanolic solvent had the highest MEY (23.48 wt%) and phenolic compounds, composed of caffeic, gallic and ferulic acids, which conferred activity against the fungus C. albicans. The solvents tested did not influence the content of soluble proteins. The solvent with 75% ethanol promoted the highest levels of glucosinolates (258.94 μmol/g) and tannins (8.80 mg/g) in the PE, reducing 96% and 98% of these contents in the PF produced. The PF obtained in the extraction with 75% ethanol contained phenolic compounds (~23 mg/100 g), dietary fibers (54.25 g/100 g) and soluble proteins (26.39 wt%), mainly composed of glutelin fraction. The PF also presented adequate functional properties, such as water solubility and absorption, which suggest potential use in pet food formulations. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

25 pages, 3669 KiB

Open AccessArticle

Impact of a Novel Two-Phase Natural Deep Eutectic Solvent-Assisted Extraction on the Structural, Functional, and Flavor Properties of Hemp Protein Isolates

by Yi Chen, Wellington S. Oliveira, Fernanda F. G. Dias and Baraem P. Ismail

Plants 2025, 14(2), 274; https://doi.org/10.3390/plants14020274 - 18 Jan 2025

Viewed by 563

Abstract

Defatting dehulled hemp seeds is a crucial step prior to protein extraction. However, conventional methods rely on flammable solvents, posing significant health, safety, and environmental concerns. Additionally, hemp protein has poor extractability, challenging functionality, and flavor limitations, restricting its broader application in foods. Accordingly, a two-phase natural deep eutectic solvent (NADES)-assisted extraction was evaluated as a solvent-free alternative for co-extracting protein and oil from full-fat hemp flour. In comparison to the reference hemp protein isolate (R-HPI), produced from hexane-defatted flour following conventional alkaline extraction, NADES-extracted hemp protein isolate (N-HPI) had significantly higher protein extraction yield and purity. N-HPI exhibited enhanced surface charge, lower hydrophobicity, and thus higher solubility at an acidic pH compared to R-HPI. N-HPI had a higher abundance of edestin and lower levels of vicilin-like proteins, which contributed to superior gelation compared to R-HPI. N-HPI, compared to R-HPI, contained lower levels of lipid-derived off-flavor compounds, such as aldehydes, alcohols, and ketones. These findings highlighted, for the first time, the potential of a two-phase NADES-assisted extraction as a sustainable alternate and effective process for producing high-quality, functional hemp protein. The development of such a green process is an impetus for broadening the applications of hemp protein in food systems. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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20 pages, 1493 KiB

Open AccessArticle

Green Extraction of Bioactives from Curcuma longa Using Natural Deep Eutectic Solvents: Unlocking Antioxidative, Antimicrobial, Antidiabetic, and Skin Depigmentation Potentials

by Jelena Jovanović, Marko Jović, Jelena Trifković, Katarina Smiljanić, Uroš Gašić, Maja Krstić Ristivojević and Petar Ristivojević

Plants 2025, 14(2), 163; https://doi.org/10.3390/plants14020163 - 8 Jan 2025

Viewed by 678

Abstract

This study evaluates the efficiency of 20 Natural Deep Eutectic Solvents (NADES) formulations for extracting curcuminoids and other bioactive compounds from turmeric and emphasize their ability to preserve and enhance antioxidant, antimicrobial, antidiabetic, and skin depigmentation effects. The NADES formulations, prepared using choline chloride (ChCl) combined with sugars, carboxylic acids, glycerol, amino acids, urea, polyols, and betaine, were assessed for their extraction efficiency based on the total phenolic content and curcumin concentration. Fourier transform infrared spectroscopy was employed to characterize the synthesized NADES and confirm their chemical composition. Bioactivity evaluations included antioxidant assays (ABTS and DPPH), antidiabetic tests (α-amylase inhibition), antimicrobial assays, and skin depigmentation (tyrosinase inhibition). The results demonstrated that NADES significantly enhanced the extraction efficiency and bioactive properties of turmeric extracts compared to water as a conventional green solvent. NADES 18 (ChCl/1,2-propanediol/water 1:1:1) and NADES 19 (glycerol/betaine/water 1:1:3) exhibited the highest extraction yields, with curcumin concentrations of 30.73 ± 1.96 mg/g and 31.70 ± 2.02 mg/g, respectively, outperforming water (26.91 ± 1.72 mg/g), while NADES 17 (ChCl/1,2-propanediol/water 0.5:3:0.5:5) and NADES 20 (glycerol/lysine/water 1:1:3) exhibited the most potent antioxidant activity. Furthermore, NADES 14 (ChCl/lactic acid/water 1:2:5) demonstrated the strongest tyrosinase inhibition (98.7%), supporting its potential for skin-brightening applications, including notable α-amylase inhibition exceeding 90%. This study aligns with the principles of green chemistry, as NADES are effective and sustainable solvents for natural product extraction. The presenting benefits of improved extraction efficiency and enhanced bioactivities position NADES as a promising and eco-friendly approach for developing efficient bioactive compound extraction methodologies. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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18 pages, 687 KiB

Open AccessArticle

Supercritical CO₂ Extraction vs. Hexane Extraction and Cold Pressing: Comparative Analysis of Seed Oils from Six Plant Species

by Katja Schoss and Nina Kočevar Glavač

Plants 2024, 13(23), 3409; https://doi.org/10.3390/plants13233409 - 4 Dec 2024

Cited by 1 | Viewed by 977

Abstract

Supercritical fluid extraction using carbon dioxide (SFE-CO₂) brings a convincing advance in the production of plant oils used in cosmetics, in fortified foods and dietary supplements, and in pharmaceuticals and medicine. The SFE-CO₂-extracted, hexane-extracted, and cold-pressed plant oils of pumpkin (Cucurbita pepo L.), flax (Linum usitatissimum L.), linden (Tilia sp.), poppy (Papaver somniferum L.), apricot (Prunus armeniaca L.), and marigold (Calendula officinalis L.) seeds were investigated in terms of oil yield, fatty acid composition, unsaponifiable matter yield and composition, and the antioxidant activity of unsaponifiable matter. SFE-CO₂ proved to be the preferred extraction method for four out of six plant materials, especially for seeds with lower oil content. However, for seeds with higher oil content, such as apricots, cold pressing is a viable alternative. A comparison of fatty acid composition did not reveal significant differences between extraction techniques. SFE-CO₂ extraction improved the total phytosterol content of oils, especially pumpkin seed oil. A high variability in the antioxidant potential of the unsaponifiable matter studied was determined, with pumpkin seed oil showing the highest antioxidant activity. A correlation analysis was performed between unsaponifiable composition and antioxidant activity, and showed statistically significant correlations with squalene, cycloartenol, and an unidentified compound. This is the first comparison of the phytosterol compositions of linseed, apricot, linden, and marigold. Through continued optimization, SFE-CO₂ has the potential to revolutionize the production of plant oils and provide a sustainable and efficient alternative. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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18 pages, 931 KiB

Open AccessArticle

Supercritical CO₂ and Conventional Extraction of Bioactive Compounds from Different Cultivars of Blackberry (Rubus fruticosus L.) Pomace

by Indrė Čechovičienė, Kiril Kazancev, Ewellina Hallmann, Eglė Sendžikienė, Marcin Kruk, Jonas Viškelis and Živilė Tarasevičienė

Plants 2024, 13(20), 2931; https://doi.org/10.3390/plants13202931 - 19 Oct 2024

Viewed by 1016

Abstract

The main objective of this work was to extract bioactive compounds from different cultivars of blackberry pomace using conventional Soxhlet and supercritical CO₂ (SC-CO₂) extraction methods. For Soxhlet extraction, two different solvents, ethanol and n-hexane, were used. Qualitative and quantitative composition of fatty acids was determined by GC, carotenoids and chlorophylls by HPLC, and volatile organic compounds were identified with an e-nose based on GC. The yield of the extract was influenced by the extraction, while the qualitative content of the extracts was also dependent on the cultivar. While there were no differences in the types of fatty acids extracted, their content varied significantly depending on the cultivar, extraction method, and their interaction. The results showed that linoleic acid (C18:2), oleic acid (C18:1), and α-linolenic acid (C18:3) were the most prevalent in all cultivars of blackberry pomace extracts. The linoleic acid content varied from 33.33 to 64.77% depending on the variety, and the ratio of omega-6 to omega-3 varied from 3.17% to 5.71%. Significantly higher quantities of carotenoids and chlorophylls were obtained in Soxhlet extraction with n-hexane in all extracts. The major carotenoid in the ‘Orkan’ and ‘Polar’ extracts was lutein, while in the ‘Brzezina’ extract, it was β-carotene. The extraction method has a significant impact on the flavor profile of the extracts. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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12 pages, 704 KiB

Open AccessArticle

Brazil Nut Semi-Defatted Flour Oil: Impact of Extraction Using Pressurized Solvents on Lipid Profile, Bioactive Compounds Composition, and Oxidative Stability

by Karen Keli Barbosa Abrantes, Tatiana Colombo Pimentel, Camila da Silva, Oscar de Oliveira Santos Junior, Carlos Eduardo Barão and Lucio Cardozo-Filho

Plants 2024, 13(19), 2678; https://doi.org/10.3390/plants13192678 - 24 Sep 2024

Viewed by 969

Abstract

Brazilian nuts are native to the Amazon rainforest and are considered a non-timber forest-product of extreme economic importance to local populations. This study evaluated the lipid profile, bioactive compounds, and oxidative stability of semi-defatted Brazilian nut flour oil (BNSDFO) obtained using pressurized fluids (n-propane at 40 °C and 2, 4, and 8 MPa or a CO₂/n-propane mixture at 40 °C and 12 MPa). A Brazilian nut kernel oil (BNKO) processed by conventional cold pressing was also obtained. The BNKO showed a higher concentration of total phenolic compounds and saturated fatty acids, higher antioxidant activity, and the presence of gallic acid derivatives. The oils extracted using pressurized fluids showed a higher concentration of linoleic acid, β-sitosterol, and polyunsaturated fatty acids. The utilization of pressurized n-propane resulted in higher yields (13.7 wt%), and at intermediate pressures (4 MPa), the product showed myricetin 3-O-rhamnoside and higher oxidative stability (OSI, 12 h) than at lower pressures (2 MPa). The CO₂/n-propane mixture of pressurized solvents resulted in higher concentrations of squalene (4.5 times), the presence of different phenolic compounds, and a high OSI (12 h) but lower yield (2.2 wt%). In conclusion, oils with better fatty acid profiles (oleic e linoleic acids), phytosterol composition, and suitable radical scavenging activity may be obtained using pressurized fluids and Brazilian nut flour, a byproduct of oil extraction. The mixture of solvents may improve the concentration of squalene, whereas using only n-propane may increase oil yield. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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14 pages, 1114 KiB

Open AccessArticle

Extraction of Bioactive Compounds from the Fruits of Jambolan (Syzygium cumini (L.)) Using Alternative Solvents

by Carla Adriana Ferrari Artilha-Mesquita, Ana Paula Stafussa, Patrícia Daniele Silva dos Santos, Oscar de Oliveira Santos, Silvio Claudio da Costa and Grasiele Scaramal Madrona

Plants 2024, 13(15), 2065; https://doi.org/10.3390/plants13152065 - 26 Jul 2024

Viewed by 1149

Abstract

This work demonstrates the effectiveness of using alternative solvents to obtain jambolan extracts with a high content of bioactive compounds compared to conventional organic solvents, being the first study to evaluate the best ecological solvent alternative for Syzygium cumini (L.) Skeels. Five alternative solvents were used for extraction: water at 25 °C (W25), water at 50 °C (W50), water at 75 °C (W75), water with citric acid at 2.4% (CA2), and water with citric acid at 9.6% (CA9) in comparison with three conventional solvents: ethanol (EtOH), water with ethanol at 50% (WE), and water with methanol at 50% (WM). A protocol was then established for the extraction and concentration of samples obtained with these solvents. The highest content of total phenolic compounds (TPCs) in the extracts was obtained with the solvent W75 (1347.27 mg GAE/100 g), while in the concentrates it was the solvents EtOH (3823.03 mg GAE/100 g) and WM (4019.39 mg GAE/100 g). Total monomeric anthocyanins (TMAs) increased by 209.31% and 179.95% in extractions with CA2 and CA9, respectively, compared to pulp (35.57 mg eq c-3-g/100 g), demonstrating that they are the most efficient alternative solvents in this extraction. The levels of bioactive compounds and antioxidant activity varied according to the solvents used. Delphinidin 3,5-diglucoside, cyanidin 3,5-diglucoside, delphinidin 3-glucoside, petunidin 3,5-diglucoside, cyanidin 3-glucoside, peonidin 3,5-diglucoside, malvidin 3,5-diglucoside, petunidin 3-glucoside, and malvidin 3-glucoside were identified in most of the samples by UPLC-MS/MS. This study suggests that a simple procedure using alternative solvents can be used as an environmentally friendly strategy to achieve efficient extraction of bioactive compounds in jambolan. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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13 pages, 1604 KiB

Open AccessArticle

Artemisia fragrans Willd. Essential Oil: Chemical Profile and Insecticidal Potential against the Confused Flour Beetle, Tribolium confusum du Val

by Asgar Ebadollahi, William N. Setzer and Franco Palla

Plants 2024, 13(13), 1725; https://doi.org/10.3390/plants13131725 - 21 Jun 2024

Cited by 1 | Viewed by 1409

Abstract

The confused flour beetle, Tribolium confusum du Val, is one of the cosmopolitan and polyphagous storage insect pests. The frequent application of chemical insecticides has resulted in several side effects, including threats to human health and non-target organisms and the resistance of insect pests. In the current study, the fumigant toxicity and feeding deterrence potential of Artemisia fragrans Willd. essential oil on T. confusum adults were investigated. The essential oil was rich in terpenic compounds, in which α-thujone (27.8%) and 1,8-cineole (22.8%) were dominant. The essential oil displayed significant fumigant toxicity on T. confusum, where a concentration of 35.3 μL/L caused 100% mortality of the treated adults after 48 h. The LC₃₀ and LC₄₀ values (lethal concentrations to kill 30% and 40% of tested insects: 15.1 and 18.4 μL/L, respectively) significantly decreased the nutritional indices of the pest, including the consumption index, relative consumption rate, and relative growth rate. The feeding deterrence index of the essential oil were calculated as being 62.29 and 48.66% for the concentrations of 15.1 and 18.4 μL/L after 5 days, respectively. Accordingly, A. fragrans essential oil can be considered an efficient, available, and natural alternative to detrimental chemical pesticides in the management of T. confusum. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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15 pages, 1858 KiB

Open AccessArticle

Optimization of the Parameters Influencing the Antioxidant Activity and Concentration of Carotenoids Extracted from Pumpkin Peel Using a Central Composite Design

by Roxana Nicoleta Gavril (Rațu), Oana Emilia Constantin, Elena Enachi, Florina Stoica, Florin Daniel Lipșa, Nicoleta Stănciuc, Iuliana Aprodu and Gabriela Râpeanu

Plants 2024, 13(11), 1447; https://doi.org/10.3390/plants13111447 - 23 May 2024

Cited by 4 | Viewed by 1910

Abstract

It has been discovered that the peel of a pumpkin (Cucurbita maxima), regarded as a waste product of pumpkin processing, has significant amounts of carotenoids and other antioxidants. This study aims to identify the most effective extraction parameters for an ultrasonic-assisted extraction method to extract the total carotenoids (TCs) and assess the antioxidant activity (AA) of pumpkin peel. To determine the effects of the extraction time, temperature, and material-to-solvent ratio on the recovery of TCs and AA, a response surface methodology utilizing the central composite design (CCD) was used. The extraction temperature (6.25–98.75 °C), extraction duration (13.98–128.98 min), and solvent ratio (0.23–50.23 mL) were the variables studied in the coded form of the experimental plan. The carotenoid concentration varied from 0.53 to 1.06 mg/g DW, while the AA varied from 0.34 to 7.28 µM TE/g DW. The findings indicated that the optimal extraction parameters were an 80 °C temperature, a 10 mL solvent ratio, and a 100 min extraction time. The study confirmed that the optimum extraction conditions resulted in an experimental TC yield of 0.97 mg/g DW and an AA of 7.25 µM TE/g DW. Overall, it should be emphasized that the extraction process can be enhanced by setting the operating factors to maximize the model responses. Full article

(This article belongs to the Special Issue Green Chemistry for Natural Product Extraction: Cleaner and Efficient Approaches)

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