Determination of Five Phthalate Esters in Tea and Their Dynamic Characteristics during Black Tea Processing
Abstract
:1. Introduction
2. Materials and Methods
2.1. Reagents and Standards for PAEs
2.2. Tea Sampling
2.3. Construction of Standard Curves of PAEs
2.4. Extraction of PAEs in Tea
2.5. Optimization of PAE Extractions in Tea Using Response Surface Methodology
2.6. GC–MS Analysis
2.7. Method Validation
2.8. Statistical Data Analysis
3. Results
3.1. Effects of Single Factors on Extraction of PAEs from Tea
3.2. Response Surface Optimization Experiment
3.3. Validation of the Developed Method
3.4. Dynamic Changes of PAEs during Black Tea Processing
4. Discussion
5. Conclusions
Supplementary Materials
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Test Number | Factor | Experimental Content (μg/kg) | Predicted Content (μg/kg) | ||
---|---|---|---|---|---|
Solid–Liquid Ratio (A) | Extraction Temperature (B) | Extraction Time (C) | |||
1 | 1:20 | 40 | 12 | 546.14 | 567.92 |
2 | 1:20 | 40 | 12 | 557.63 | 576.48 |
3 | 1:10 | 50 | 12 | 348.29 | 328.23 |
4 | 1:20 | 40 | 12 | 647.50 | 585.85 |
5 | 1:20 | 40 | 12 | 559.27 | 577.11 |
6 | 1:20 | 40 | 12 | 529.08 | 533.45 |
7 | 1:10 | 40 | 18 | 416.98 | 402.39 |
8 | 1:30 | 30 | 12 | 216.75 | 236.81 |
9 | 1:20 | 30 | 6 | 193.37 | 158.72 |
10 | 1:20 | 50 | 18 | 395.63 | 430.28 |
11 | 1:10 | 30 | 12 | 219.02 | 249.49 |
12 | 1:10 | 40 | 6 | 166.01 | 170.17 |
13 | 1:30 | 50 | 12 | 302.30 | 207.11 |
14 | 1:30 | 40 | 6 | 138.57 | 153.16 |
15 | 1:20 | 30 | 18 | 380.81 | 364.92 |
16 | 1:30 | 40 | 18 | 354.47 | 350.30 |
17 | 1:20 | 50 | 6 | 191.22 | 207.11 |
Source of Variance | Degrees of Freedom | Sum of Square | Mean Square | F-Value | p-Value | Distinctiveness |
---|---|---|---|---|---|---|
A-Solid–liquid ratio | 1 | 2387.40 | 2387.40 | 1.15 | 0.3190 | |
B-Extraction temperature | 1 | 6468.96 | 6468.96 | 3.12 | 0.1208 | |
C-Extraction time | 1 | 92,177.15 | 92,177.15 | 44.42 | 0.0003 | ** |
AB | 1 | 477.86 | 477.86 | 0.23 | 0.6459 | |
AC | 1 | 307.65 | 307.65 | 0.15 | 0.7116 | |
BC | 1 | 72.00 | 72.00 | 0.035 | 0.8575 | |
A2 | 1 | 1.062 × 105 | 1.062 × 105 | 51.16 | 0.0002 | ** |
B2 | 1 | 79,652.45 | 79,652.45 | 38.39 | 0.0004 | ** |
C2 | 1 | 82,674.64 | 82,674.64 | 39.84 | 0.0004 | ** |
Model | 9 | 4.018 × 105 | 44,642.87 | 21.51 | 0.0003 | ** |
Residual | 7 | 14,525.52 | 2075.07 | |||
Lack-of-fit | 3 | 6028.92 | 2009.64 | 0.95 | 0.4980 | |
Pure error | 4 | 8496.60 | 2124.15 | |||
Cor total | 16 | 4.163 × 105 |
Number | Compound | Retention Time (min) | Qualitativeion (m/z) | Quantitative Ion (m/z) |
---|---|---|---|---|
1 | DMP | 12.98 | 163,77,194,133 | 163 |
2 | DEP | 17.38 | 149,177,105,222 | 149 |
3 | DiBP | 26.90 | 149,223,104,167 | 149 |
4 | DBP | 29.50 | 149,223,205,104 | 149 |
5 | DEHP | 39.57 | 149,167,279,113 | 149 |
PAEs | Linear Range (μg/L) | r2 | LOD (μg/kg) | LOQ (μg/kg) | Recoveries, % (RSD, %) | Matrix Effect | ||
---|---|---|---|---|---|---|---|---|
100 μg/L | 500 μg/L | 1000 μg/L | ||||||
DMP | 1.00–1000.00 | 0.9910 | 0.40 | 1.33 | 81.71 (4.32) | 95.00 (7.55) | 97.07 (5.70) | 1.13 |
DEP | 1.00–1000.00 | 0.9914 | 0.61 | 2.03 | 80.70 (5.60) | 94.28 (6.52) | 93.88 (4.56) | 1.02 |
DIBP | 1.00–1000.00 | 0.9950 | 0.42 | 1.40 | 82.69 (8.14) | 94.22 (4.03) | 91.57 (3.31) | 0.63 |
DBP | 1.00–500.00 | 0.9961 | 0.50 | 1.66 | 89.30 (6.67) | 90.37 (8.69) | 98.28 (4.58) | 0.50 |
DEHP | 1.00–1000.00 | 0.9963 | 0.21 | 0.71 | 84.37 (6.39) | 93.99 (3.94) | 98.68 (2.72) | 0.40 |
Sample | DMP | DEP | DIBP | DBP | DEHP | Sum |
---|---|---|---|---|---|---|
Fresh leaves sample | 12.31 ± 0.39 | 35.13 ± 0.17 | 33.15 ± 0.56 | 430.41 ± 15.08 | 16.89 ± 1.64 | 527.90 ± 31.38 |
Withered sample | 11.36 ± 0.35 | 13.01 ± 0.22 | 21.73 ± 0.37 | 1436.37 ± 17.32 | 24.73 ± 2.29 | 1507.21 ± 139.04 |
Rolled sample | 11.28 ± 0.87 | 12.97 ± 0.51 | 22.68 ± 1.34 | 1166.90 ± 18.83 | 26.86 ± 3.99 | 1240.86 ± 109.02 |
Fermented sample | 11.44 ± 0.39 | 12.87 ± 0.54 | 19.13 ± 1.88 | 895.98 ± 9.16 | 23.56 ± 1.69 | 962.97 ± 100.84 |
First drying sample | 11.67 ± 0.40 | 12.99 ± 0.33 | 20.77 ± 1.37 | 1313.84 ± 9.31 | 28.33 ± 1.52 | 1387.61 ± 128.37 |
Finished tea sample | 11.26 ± 1.47 | 12.82 ± 2.68 | 37.08 ± 3.87 | 387.69 ± 4.09 | 11.73 ± 1.72 | 460.85 ± 4.33 |
PAEs | CAS Number | Mw | Log Kow | Sw (mg/L, 25 °C) | Vp (mm Hg, 25 °C) | Mp (°C) | Bp (°C) | Structural Formula |
---|---|---|---|---|---|---|---|---|
DMP | 131-11-3 | 194.19 | 1.60 | 4000.00 | 3.08 × 10−3 | 5.50 | 282.68 | |
DEP | 84-66-2 | 222.24 | 2.42 | 1080.00 | 2.10 × 10−3 | −40.50 | 294.00 | |
DiBP | 84-69-5 | 278.35 | 4.11 | 6.20 | 4.76 × 10−5 | −50.00 | 327.00 | |
DBP | 84-74-2 | 278.35 | 4.50 | 11.20 | 2.01 × 10−5 | −35.00 | 337.00 | |
DEHP | 117-81-7 | 390.57 | 7.60 | 0.27 | 1.42 × 10−7 | −50.00 | 384.90 |
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Tang, Y.; Wang, M.; Pan, C.; Mi, S.; Han, B. Determination of Five Phthalate Esters in Tea and Their Dynamic Characteristics during Black Tea Processing. Foods 2022, 11, 1266. https://doi.org/10.3390/foods11091266
Tang Y, Wang M, Pan C, Mi S, Han B. Determination of Five Phthalate Esters in Tea and Their Dynamic Characteristics during Black Tea Processing. Foods. 2022; 11(9):1266. https://doi.org/10.3390/foods11091266
Chicago/Turabian StyleTang, Yanyan, Mengxin Wang, Cheng Pan, Shuishan Mi, and Baoyu Han. 2022. "Determination of Five Phthalate Esters in Tea and Their Dynamic Characteristics during Black Tea Processing" Foods 11, no. 9: 1266. https://doi.org/10.3390/foods11091266