Human Exposure to Chlorinated Organophosphate Ester Flame Retardants and Plasticizers in an Industrial Area of Shenzhen, China
Abstract
:1. Introduction
2. Materials and Methods
2.1. Sample Collection
2.2. Standards and Reagents
2.3. Sample Pretreatment and Instrumental Analysis
2.4. Quality Assurance and Quality Control
2.5. Heath Risk Assessment
2.6. Data Analyses
3. Results and Discussion
3.1. Concentrations and Profiles of OPEs in Urine and Plasma Sample
3.2. MOPEs in Plasma and Recommendations for Biomarkers
3.3. Global and Regional Comparison of OPEs and Health Risk Assessment
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
Appendix A
Category | Number (Percentage) | |
---|---|---|
Age | <18 | 6 (11.76%) |
18–44 | 37 (72.55%) | |
45–59 | 7 (13.73%) | |
>59 | 1 (1.96%) | |
Gender | Male | 12 (23.53%) |
Female | 39 (76.47%) |
No. | Compound | Abbreviation | Molecular Formula | CAS No. | Manufacturers |
---|---|---|---|---|---|
1 | Tris(2-butoxyethyl) phosphate | TBOEP | C18H39O7P | 78-51-3 | Dr. Ehrenstorfer GmbH (Augsburg, Germany) |
2 | Trimethyl phosphate | TMP | C3H9O4P | 512-56-1 | AccuStandard (New Haven, CT, USA) |
3 | Tri-n-butyl phosphate | TnBP | C12H27O4P | 126-73-8 | Dr. Ehrenstorfer GmbH (Augsburg, Germany) |
4 | 2-Ethylhexyl diphenyl phosphate | EHDPP | C20H27O4P | 1241-94-7 | |
5 | Tri-iso-butyl phosphate | TIBP | C12H27O4P | 126-71-6 | ANPEL Laboratory Technologies Inc. (Shanghai, China) |
6 | Triethyl phosphate | TEP | C6H15O4P | 78-40-0 | AccuStandard (New Haven, CT, USA) |
7 | Tetraphenyl m-phenylene bis(phosphate) | RDP | C30H20O8P2 | 57583-54-7 | |
8 | Tripentyl phosphate | TNP | C15H33O4P | 2528-38-3 | |
9 | Tripropyl phosphate | TPrP | C9H21O4P | 513-08-6 | Dr. Ehrenstorfer GmbH (Augsburg, Germany) |
10 | Triphenyl phosphate | TPHP | C18H15O4P | 115-86-6 | |
11 | Triphenylphosphine Oxide | TPPO | C18H15OP | 791-28-6 | Toronto Research Chemicals Inc. (Toronto, ON, Canada) |
12 | Cresyl Diphenyl Phosphate | CDP | C19H17O4P | 26444-49-5 | Dr. Ehrenstorfer GmbH (Augsburg, Germany) |
13 | Tris(2-ethylhexyl) phosphate | TEHP | C24H51O4P | 78-42-2 | |
14 | Tris(2-chloropropyl) phosphate | TCPP | C9H18CL3PO4 | 13674-84-5 | AccuStandard (New Heavn, CT, USA) |
15 | Tris(1,3-dichloro-2-propyl) phosphate | TDCIPP | C9H15Cl6O4P | 13674-87-8 | |
16 | Tris(2-chloroethyl) phosphate | TCEP | C6H12Cl3O4P | 115-96-8 | Dr. Ehrenstorfer GmbH (Augsburg, Germany) |
17 | Triisopropyl phosphate | TiPrP | C9H21O4P | 513-02-0 | AccuStandard (New Heavn, CT, USA) |
18 | Diethyl phosphate | DEP | C4H11O4P | 598-02-7 | |
19 | Di-n-butyl phosphate | DnBP | C8H19O4P | 107-66-4 | Dr. Ehrenstorfer GmbH (Augsburg, Germany) |
20 | Bis(2-butoxyethyl)2-hydroxyethyl phosphate triester | BBOEHP | C14H31O7P | 1477494-86-2 | Toronto Research Chemicals Inc. (Toronto, ON, Canada) |
21 | Bis(butoxyethyl)phosphate | BBOEP | C12H27O6P | 14260-97-0 | |
22 | Bis(2-butoxyethyl)2-(3-hydroxybutoxy)ethyl phosphate ttriester | 3-OH-TBOEP | C18H39O8P | 1477494-87-3 |
Time (min) | Mobile Phase A (%) | Mobile Phase B (%) |
---|---|---|
0 | 30 | 70 |
2 | 60 | 40 |
22 | 85 | 15 |
24 | 98 | 2 |
25 | 98 | 2 |
30 | 30 | 70 |
Analyte | Precursor Ion (m/z) | Fragment (V) | Product Ion (m/z) | CE (V) |
---|---|---|---|---|
TBOEP | 399 | 124 | 45/57 | 25/37 |
TMP | 141 | 96 | 109/47 | 17/29 |
TnBP | 267 | 81 | 99/211 | 13/5 |
EHDPP | 251 | 117 | 51/77 | 69/33 |
TIBP | 267 | 81 | 99/81 | 13/61 |
TEP | 183 | 61 | 99/81 | 17/49 |
RDP | 575 | 210 | 77/152 | 85/70 |
TNP | 309 | 101 | 99/81 | 17/77 |
TPrP | 225 | 76 | 99/141 | 13/5 |
TPHP | 327 | 157 | 77/152 | 49/45 |
TPPO | 279 | 170 | 201/77 | 25/53 |
CDP | 341 | 175 | 91/65 | 37/73 |
TEHP | 434 | 130 | 99/113 | 40/10 |
TCPP | 327 | 100 | 99/175 | 18/10 |
TDCIPP | 431 | 110 | 99/209 | 15/12 |
TCEP | 285 | 85 | 99/63 | 20/26 |
TiPrP | 225 | 64 | 99/81 | 13/57 |
DEP | 155 | 75 | 99/127 | 13/5 |
DnBP | 211 | 75 | 99/63 | 9/89 |
BBOEHP | 343 | 95 | 45/243 | 17/9 |
BBOEP | 299 | 95 | 45/199 | 17/9 |
3-OH-TBOEP | 415 | 105 | 45/55 | 25/37 |
TBOEP-d27 | 426 | 105 | 46/66 | 25/37 |
TMP-C13 | 144 | 90 | 111/80 | 20/40 |
TnBP-d27 | 294 | 95 | 102/83 | 17/77 |
Analyte | Recoveries | Urine | Plasma | |||
---|---|---|---|---|---|---|
Urine | Plasma | MDLs | MQLs | MDLs | MQLs | |
TBOEP | 85.4 ± 20.3 | 86.9 ± 14.4 | 0.05 | 0.2 | 0.2 | 0.8 |
TMP | 82.3 ± 17.4 | 84.3 ± 12.1 | 0.05 | 0.2 | 0.2 | 0.8 |
TnBP | 76.5 ± 10.4 | 86.1 ± 15.3 | 0.05 | 0.2 | 0.2 | 0.8 |
EHDPP | 91.0 ± 22.6 | 79.6 ± 13.4 | 0.1 | 0.4 | 0.4 | 1.5 |
TIBP | 84.8 ± 17.4 | 84.5 ± 16.7 | 0.05 | 0.2 | 0.2 | 0.8 |
TEP | 93.1 ± 20.2 | 83.1 ± 18.3 | 0.1 | 0.4 | 0.4 | 1.5 |
RDP | 85.6 ± 18.8 | 89.2 ± 22.6 | 0.2 | 0.8 | 0.8 | 3 |
TNP | 79.5 ± 12.9 | 76.8 ± 12.6 | 0.1 | 0.4 | 0.4 | 1.5 |
TPrP | 86.7 ± 21.3 | 87.9 ± 23.7 | 0.02 | 0.08 | 0.1 | 0.4 |
TPHP | 89.6 ± 20.8 | 89.7 ± 19.5 | 0.02 | 0.08 | 0.1 | 0.4 |
TPPO | 68.3 ± 10.1 | 86.1 ± 15.3 | 0.05 | 0.2 | 0.2 | 0.8 |
CDP | 78.8 ± 15.5 | 90.3 ± 23.2 | 0.2 | 0.8 | 0.8 | 3 |
TEHP | 73.8 ± 16.2 | 86.8 ± 16.2 | 0.1 | 0.4 | 0.4 | 1.5 |
TCPP | 76.2 ± 8.6 | 91.8 ± 21.3 | 0.2 | 0.8 | 0.8 | 3 |
TDCIPP | 81.1 ± 15.2 | 103.2 ± 16.8 | 0.3 | 1 | 1 | 4 |
TCEP | 103.1 ± 23.2 | 107.3 ± 24.0 | 0.3 | 1 | 1 | 4 |
TiPrP | 79.2 ± 16.6 | 84.9 ± 14.3 | 0.02 | 0.08 | 0.08 | 0.4 |
DEP | 89.3 ± 13.3 | 89.1 ± 8.3 | 0.08 | 0.3 | 0.3 | 1 |
DnBP | 76.3 ± 5.6 | 79.3 ± 5.4 | 0.05 | 0.2 | 0.2 | 0.8 |
BBOEHP | 87.2 ± 7.9 | 76.8.4 ± 3.6 | 0.05 | 0.2 | 0.2 | 0.8 |
BBOEP | 78.4 ± 14.3 | 82.6 ± 11.3 | 0.05 | 0.2 | 0.2 | 0.8 |
3-OH-TBOEP | 84.5 ± 15.2 | 82.9 ± 12.6 | 0.04 | 0.15 | 0.15 | 0.6 |
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DF(%) | Median | Mean | Geometric Mean | Standard Deviation | Min | Max | |
---|---|---|---|---|---|---|---|
Urine Samples (n = 30) | |||||||
TCPP | 90 | 1.35 | 1.52 | 1.07 | 0.99 | n.d. | 4.79 |
TCEP | 50 | n.d. | 3.37 | 0.47 | 5.19 | n.d. | 15.82 |
TBOEP | 63.33 | 0.26 | 0.51 | 0.12 | 0.84 | n.d. | 3.41 |
EHDPP | 6.67 | n.d. | 0.60 | n.d. | 0.1 | n.d. | 0.67 |
Plasma Samples (n = 21) | |||||||
TCPP | 100 | 17.21 | 17.09 | 15.89 | 6.49 | 7.27 | 29.92 |
TCEP | 28.57 | n.d. | 3.79 | n.d. | 6.5 | n.d. | 17.77 |
TEP | 85.71 | 4.85 | 4.64 | 3.59 | 2.18 | n.d. | 8.04 |
TPPO | 4.76 | n.d. | n.d. | n.d. | - | n.d. | 12.68 |
Parent OPEs | DF (%) | Mean (Min–Max) | mOPEs | Properties | DF (%) | Mean (Min–Max) |
---|---|---|---|---|---|---|
TnBP | 0 | n.d. | Di-n-butyl phosphate(DnBP) | Dialkyl metabolites | 85.71 | 8.22 (n.d.–13.78) |
TEP | 85.71 | 4.64 (n.d.–8.04) | Diethyl phosphate(DEP) | 52.38 | 2.29 (n.d.–9.96) | |
TBOEP | 0 | n.d. | Bis(2-butoxyethyl) phosphate (BBOEP) | Dialkyl metabolites | 0 | n.d. |
Bis(2-butoxyethyl)2-hydroxyethyl phosphate trimester (BBOEHP) | Hydroxylated metabolites | 0 | n.d. | |||
Bis(2-butoxyethyl)2-(3-hydroxybutoxy)ethyl phosphate trimester (3-OH-TBOEP) | 0 | n.d. |
Region | Time | TCEP | TCIPP | TDCPP | TPHP | TEP | TBOEP | EHDPP | Reference |
---|---|---|---|---|---|---|---|---|---|
Urine (Geometric Mean, ng/mL) | |||||||||
Shenzhen, China | 2020 | 0.47 | 1.07 | n.d | n.d | n.d | 0.12 | n.d | This study |
Beijing, China | 2018 | n.d | n.d | n.d | n.d | 0.075 | 0.038 | n.d | [14] |
Hongkong, China | 2016 | 0.015 | 0.021 | 0.06 | 0.46 | - | - | 0.54 | [28] |
Jinan, China | 2018 | 0.298 | 0.743 | - | 0.4 | - | - | 0.209 | [24] |
Australia | 2014 | n.d | n.d | n.d | n.d | n.d | n.d | n.d | [29] |
Australia | 2015 | n.d | n.d | 0.024 | - | - | 0.59 | n.d | [30] |
Blood/Serum or Plasma (Median, ng/mL) | |||||||||
Shenzhen, China | 2020 | n.d | 17.21 | n.d | n.d | 4.85 | n.d | n.d | This study |
Shenzhen, China | 2012 | n.d | 0.71 | n.d. | 0.43 | 0.49 | 0.54 | 1.22 | [5] |
Hebei, China | 2017 | 0.18 | 0.25 | n.d | 0.46 | - | n.d. | 0.78 | [31] |
Jinan, China | 2018 | 0.3 | 0.74 | 0.11 | 0.4 | 0.14 | - | 0.21 | [24] |
Beijing, China | 2018 | n.d | n.d | n.d | 0.37 | 0.43 | 0.16 | 1.1 | [14] |
Jiangsu, China | 2013 | 0.1 | 0.05 | n.d | 0.35 | 0.15 | 0.05 | 0.85 | [32] |
Shandong, China | 2018 | 214 | n.d. | - | - | n.d. | - | 7.2 | [33] |
Spain | 2016 | 3.69 | 93.9 | n.d. | 22.7 | n.d. | 56.4 | 425.8 | [34] |
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Liu, Y.; Zhu, T.; Xie, Z.; Deng, C.; Qi, X.; Hu, R.; Wang, J.; Chen, J. Human Exposure to Chlorinated Organophosphate Ester Flame Retardants and Plasticizers in an Industrial Area of Shenzhen, China. Int. J. Environ. Res. Public Health 2022, 19, 3126. https://doi.org/10.3390/ijerph19053126
Liu Y, Zhu T, Xie Z, Deng C, Qi X, Hu R, Wang J, Chen J. Human Exposure to Chlorinated Organophosphate Ester Flame Retardants and Plasticizers in an Industrial Area of Shenzhen, China. International Journal of Environmental Research and Public Health. 2022; 19(5):3126. https://doi.org/10.3390/ijerph19053126
Chicago/Turabian StyleLiu, Yunlang, Tingting Zhu, Zuoming Xie, Chen Deng, Xiujuan Qi, Rong Hu, Jinglin Wang, and Jianyi Chen. 2022. "Human Exposure to Chlorinated Organophosphate Ester Flame Retardants and Plasticizers in an Industrial Area of Shenzhen, China" International Journal of Environmental Research and Public Health 19, no. 5: 3126. https://doi.org/10.3390/ijerph19053126