Green Valorization of Olive Leaves to Produce Polyphenol-Enriched Extracts Using an Environmentally Benign Deep Eutectic Solvent
Abstract
:1. Introduction
2. Materials and Methods
2.1. Chemicals
2.2. Collection of Plant Material and Handling
2.3. Synthesis of DES
2.4. Batch Stirred-Tank Extraction
2.5. Design of Experiment—Response Surface Methodology
2.6. Total Polyphenol Determination
2.7. Total Flavonoid Determination
2.8. Antiradical Activity (AAR) Determination
2.9. Ferric-Reducing Power (PR) Determination
2.10. Liquid Chromatography-Diode Array-Mass Spectrometry (LC-DAD-MS)
2.11. High-Performance Liquid Chromatography (HPLC)
2.12. Statistical Analysis
3. Results and Discussion
3.1. Effect of DES Composition
3.2. Extraction Process Optimization
3.3. Temperature Effects
3.4. Polyphenolic Composition
4. Conclusions
Author Contributions
Funding
Conflicts of Interest
Nomenclature
AAR | antiradical activity (μmol DPPH g−1) |
CDES | proportion of DES/water (%, w/v) |
PR | reducing power (μmol AAE g−1) |
RL/S | liquid-to-solid ratio (mL g−1) |
SS | stirring speed (rpm) |
t | time (min) |
T | temperature (°C) |
YTFn | yield in total flavonoids (mg RtE g−1) |
YTP | yield in total polyphenols (mg GAE g−1) |
Abbreviations
AAE | ascorbic acid equivalents |
DPPH | 2,2-diphenyl-1-picrylhydrazyl radical |
GAE | gallic acid equivalents |
Gly | glycine |
HBA | hydrogen bond acceptor |
LA | lactic acid |
OLL | olive leaves |
TPTZ | 2,4,6-tripyridyl-s-triazine |
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Independent Variables | Code Units | Coded Variable Level | ||
---|---|---|---|---|
−1 | 0 | 1 | ||
CDES (%, w/v) | X1 | 55 | 70 | 85 |
RL/S (mL g−1) | X2 | 20 | 40 | 60 |
SS (rpm) | X3 | 200 | 500 | 800 |
Solvent | YTP (mg GAE g−1 dm) | YTFn (mg RtE g−1 dm) | AAR (μmol DPPH g−1 dm) | PR (μmol AAE g−1 dm) |
---|---|---|---|---|
Water | 46.64 ± 2.80 | 7.81 ± 0.47 | 265.93 ± 5.32 | 213.15 ± 3.20 |
60% MeOH | 79.23 ± 4.75 | 18.33 ± 1.10 | 381.17 ± 7.62 | 276.26 ± 4.14 |
60% EtOH | 76.07 ± 4.56 | 22.12 ± 1.33 | 347.93 ± 6.96 | 265.43 ± 3.98 |
LA-Gly (5:1) a | 93.73 ± 5.16 * | 17.28 ± 0.95 | 508.60 ± 10.17 * | 400.61 ± 6.01 * |
Term | Standard Error | t Ratio | Probability > t | Sum of Squares | F Ratio |
---|---|---|---|---|---|
CDES | 0.901165 | 5.44 | 0.0029* | 192.17801 | 29.5805 |
RL/S | 0.901165 | −4.85 | 0.0047* | 152.68781 | 23.5020 |
SS | 0.901165 | −0.78 | 0.4694 | 3.97620 | 0.6120 |
CDES RL/S | 1.27444 | −0.78 | 0.4682 | 4.00000 | 0.6157 |
CDES SS | 1.27444 | −0.24 | 0.8218 | 0.36602 | 0.0563 |
RL/S SS | 1.27444 | −3.13 | 0.0259 * | 63.76023 | 9.8141 |
CDESCDES | 1.326479 | −3.61 | 0.0154 * | 84.74616 | 13.0443 |
RL/S RL/S | 1.326479 | −8.90 | 0.0003 * | 514.62536 | 79.2123 |
SS SS | 1.326479 | −2.41 | 0.0611 | 37.65186 | 5.7955 |
Lack-of-fit | 0.3241 | 32.483942 | 2.2340 |
Design Point | Independent Variables | Response (YTP, mg GAE g−1 dm) | |||
---|---|---|---|---|---|
X1 (CDES, % w/v) | X2 (RL/S, mL g−1) | X3 (SS, rpm) | Measured | Predicted | |
1 | −1 (55) | −1 (20) | 0 (500) | 79.88 | 77.64 |
2 | −1 (55) | 1 (60) | 0 (500) | 71.67 | 70.90 |
3 | 1 (85) | −1 (20) | 0 (500) | 88.67 | 89.44 |
4 | 1 (85) | 1 (60) | 0 (500) | 76.46 | 78.70 |
5 | 0 (70) | −1 (20) | −1 (200) | 80.55 | 81.85 |
6 | 0 (70) | −1 (20) | 1 (800) | 88.25 | 88.42 |
7 | 0 (70) | 1 (60) | −1 (200) | 81.27 | 81.10 |
8 | 0 (70) | 1 (60) | 1 (800) | 73.00 | 71.70 |
9 | −1 (55) | 0 (40) | −1 (200) | 82.34 | 83.28 |
10 | 1 (85) | 0 (40) | −1 (200) | 95.76 | 93.69 |
11 | −1 (55) | 0 (40) | 1 (800) | 80.41 | 82.48 |
12 | 1 (85) | 0 (40) | 1 (800) | 92.62 | 91.68 |
13 | 0 (70) | 0 (40) | 0 (500) | 93.54 | 95.77 |
14 | 0 (70) | 0 (40) | 0 (500) | 97.00 | 95.77 |
15 | 0 (70) | 0 (40) | 0 (500) | 96.76 | 95.77 |
T (° C) | YTP (mg GAE g−1 dm) | YTFn (mg RtE g−1 dm) | AAR (μmol DPPH g−1 dm) | PR (μmol AAE g−1 dm) |
---|---|---|---|---|
50 | 96.41 ± 2.27 | 19.47 ± 0.68 | 637.14 ± 11.57 | 407.00 ± 7.00 |
80 | 98.77 ± 2.00 | 26.44 ± 0.98 | 773.21 ± 13.89 | 461.18 ± 8.11 |
Polyphenol | Content (mg g−1 dm) ± sd |
---|---|
Hydroxytyrosol | 8.20 ± 0.12 |
Rutin | 0.28 ± 0.00 |
Luteolin 7-O-glucoside | 2.59 ± 0.04 |
Apigenin 7-O-rutinoside | 0.36 ± 0.01 |
Luteolin 3’-O-glucoside | 0.36 ± 0.01 |
Oleuropein | 2.88 ± 0.04 |
Quercetin | 0.44 ± 0.01 |
Apigenin | 0.01 ± 0.00 |
Sum | 15.13 |
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Kaltsa, O.; Grigorakis, S.; Lakka, A.; Bozinou, E.; Lalas, S.; Makris, D.P. Green Valorization of Olive Leaves to Produce Polyphenol-Enriched Extracts Using an Environmentally Benign Deep Eutectic Solvent. AgriEngineering 2020, 2, 226-239. https://doi.org/10.3390/agriengineering2020014
Kaltsa O, Grigorakis S, Lakka A, Bozinou E, Lalas S, Makris DP. Green Valorization of Olive Leaves to Produce Polyphenol-Enriched Extracts Using an Environmentally Benign Deep Eutectic Solvent. AgriEngineering. 2020; 2(2):226-239. https://doi.org/10.3390/agriengineering2020014
Chicago/Turabian StyleKaltsa, Olga, Spyros Grigorakis, Achillia Lakka, Eleni Bozinou, Stavros Lalas, and Dimitris P. Makris. 2020. "Green Valorization of Olive Leaves to Produce Polyphenol-Enriched Extracts Using an Environmentally Benign Deep Eutectic Solvent" AgriEngineering 2, no. 2: 226-239. https://doi.org/10.3390/agriengineering2020014