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1.
Environ Res ; 252(Pt 1): 118768, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38521355

RESUMEN

Chlorinated paraffins (CPs) are hazardous to humans, and dietary intake acts as the primary pathway for human exposure to CPs. Takeout food is popular worldwide, but the presence of CPs in takeout food and its packaging is unclear. In this study, the concentrations and distributions of short- and median-chain CPs (SCCPs and MCCPs, respectively) were measured in 97 samples of four categories of takeout food and 33 samples of three types of takeout packaging. The SCCP and MCCP median concentrations for the takeout food samples were 248 and 339, 77.2 and 98.2, 118 and 258, 42.9 and 64.4 ng/g wet weight in meat, starch, half meat/half starch, and vegetables, respectively. Takeout food contained higher concentrations of SCCPs than MCCPs. The dominant SCCP and MCCP congener groups in takeout food were C10Cl6-7 and C14Cl7-8, respectively. The CP concentrations in takeout food were lower than those in packaging. The SCCP and MCCP median concentrations, respectively, in packaging were 9750 and 245 ng/g in polypropylene, 2830 and 135 ng/g in paper, and 2060 and 119 ng/g in aluminum foil. The concentrations of SCCPs and MCCPs were comparable in aluminum foil, whereas the concentrations of SCCPs were higher than those of MCCPs in polypropylene and paper. Correlations between CP concentrations in the takeout food and packaging indicated that CPs in packaging were potentially an important source of CPs in the takeout food. A dietary exposure risk assessment showed the takeout food posed a low risk for human exposure to CPs; however, high-frequency consumption may pose a health risk. This study clarified the current contamination situation in takeout food in Beijing, China. The resulting data could be used to prevent human exposure to CPs through dietary intake and to facilitate the market's control over the quality of takeout food.


Asunto(s)
Exposición Dietética , Contaminación de Alimentos , Embalaje de Alimentos , Parafina , Exposición Dietética/análisis , Contaminación de Alimentos/análisis , Parafina/análisis , Humanos , Medición de Riesgo , Beijing , Hidrocarburos Clorados/análisis , China
2.
Environ Sci Technol ; 57(45): 17522-17533, 2023 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-37905521

RESUMEN

Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and short-chain chlorinated paraffins (SCCPs) can be formed during the production of chlorinated paraffins (CPs). Detection and accurate quantification of PCDD/Fs in CPs are challenging because of their matrix complexity. Therefore, the occurrence and formation mechanisms of PCDD/Fs from CPs have not been studied extensively in the past. In this study, 15 commercial samples including solid and liquid CPs were collected in 2022 from China. The average ΣSCCP concentrations detected in the solid and liquid CPs were 158 and 137 mg/g, respectively. The average International Toxic Equivalent (I-TEQ) values of 2,3,7,8-PCDD/F in solid and liquid CPs were 15.8 pg I-TEQ/g and 15.0 pg I-TEQ/g, respectively. The solid and liquid CPs had different predominant congener groups for SCCPs and PCDD/Fs. Possible formation routes for the generation of PCDD/Fs were analyzed by screening precursors in paraffin and laboratory-scale thermochemical experiments of CPs. The transformation between 2,3,7,8-PCDD/Fs and non-2,3,7,8-PCDD/Fs was recognized by calculating the successive chlorination preference. The first reported occurrence of PCDD/Fs in CP commercial products indicated that exposure to CPs and downstream products might be an assignable source of PCDD/F emission, which is of great significance to further explore the control factors of PCDD/Fs in the whole life cycle of CPs.


Asunto(s)
Benzofuranos , Dioxinas , Dibenzodioxinas Policloradas , Parafina , Dibenzofuranos , Dibenzofuranos Policlorados/análisis , Benzofuranos/análisis , Aceite Mineral , China , Monitoreo del Ambiente
3.
Environ Geochem Health ; 45(7): 4631-4642, 2023 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-36881246

RESUMEN

Chlorinated paraffins (CPs), a group of mixtures with different carbon chain lengths and chlorine contents, are widely used as plasticizers and flame retardants in various indoor materials. CPs could be released from CP-containing materials into the ambient environment and then enter the human body via inhalation, dust ingestion and dermal absorption, resulting in potential effects on human health. In this study, we collected residential indoor dust in Wuhan, the largest city in central China, and focused on the co-occurrence and composition profiles of CPs as well as the resultant human risk via dust ingestion and dermal absorption. The results indicated that CPs with C9-40 were ubiquity in indoor dust with medium-chain CPs (MCCPs, C14-17) as the main components (6.70-495 µg g-1), followed by short-chain CPs (SCCPs, C10-13) (4.23-304 µg g-1) and long-chain (LCCPs, C≥18) CPs (3.68-331 µg g-1). Low levels (not detected-0.469 µg g-1) of very short-chain CPs (vSCCPs, C9) were also found in partial indoor dust. The dominant homolog groups were C9 and Cl6-7 groups for vSCCPs, C13 and Cl6-8 groups for SCCPs, C14 and Cl6-8 groups for MCCPs, and C18 and Cl8-9 groups for LCCPs. Based on the measured concentrations, vSCCPs, SCCPs, MCCPs, and LCCPs posed limited human health risks to local residents via dust ingestion and dermal absorption.


Asunto(s)
Contaminación del Aire Interior , Hidrocarburos Clorados , Humanos , Polvo/análisis , Monitoreo del Ambiente/métodos , Parafina/análisis , Hidrocarburos Clorados/análisis , Contaminación del Aire Interior/análisis , China
4.
J Hazard Mater ; 455: 131640, 2023 08 05.
Artículo en Inglés | MEDLINE | ID: mdl-37201278

RESUMEN

Chlorinated paraffins (CPs) are emerging environmental pollutants. Although metabolism has been shown to affect the differential accumulation of short-chain (SCCPs), medium-chain (MCCPs) and long-chain (LCCPs) CPs in birds, CP metabolites have rarely been reported and the extent to which they are formed is still unclear. In this study, single and mixed CP standards were incubated with chicken liver microsomes in vitro to study the generation of CP metabolites. Putative aldehyde/ketone and carboxylic acid metabolites identified by mass spectroscopy data were shown to be false positive results. Phase I metabolism of CPs first formed monohydroxylated ([M-Cl+OH]) and then dihydroxylated ([M-2Cl+2OH]) products. The yields of monohydroxylated metabolites of CPs decreased with increasing carbon chain length and chlorine content at the initial stage of reaction. Notably, the yield of monohydroxylated metabolites of SCCPs with 51.5% Cl content reached 21%, and that of 1,2,5,6,9,10-hexachlorodecane (C10H16Cl6) was as high as 71%. Thus, monohydroxy metabolites of CPs in birds should not be ignored, especially those of SCCPs. This study provides important data that could support improvements to the ecological/health risk assessment of CPs.


Asunto(s)
Hidrocarburos Clorados , Animales , Hidrocarburos Clorados/análisis , Microsomas Hepáticos , Parafina/química , Pollos , Monitoreo del Ambiente/métodos , China
5.
Environ Sci Pollut Res Int ; 30(56): 119450-119461, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37924406

RESUMEN

Short-chain chlorinated paraffins (SCCPs) are listed in the Stockholm Convention. Therefore, selecting suitable methods for their accurate quantification is essential. Nowadays, the quality of commercial reagents employed as quantification standards is not guaranteed. As a solution, we adopted an SCCP formulation reference material with known homolog composition ratios as the quantification standard to evaluate the appropriateness of the methods. By mixing the SCCP formulation and interferences, an analytical sample was independently prepared and used as the simulation environmental sample. The homolog compositional profiles of the SCCPs resembled those of the quantification standard and the analytical sample. The mass fractions and the homolog profiles, including the carbon chain length and chlorine homolog profiles, of the SCCPs were reported by 14 different laboratories. For the mass fraction, the results reported by participants were consistent, except for the participants that employed low-resolution gas chromatography (GC). The results generated from liquid chromatography (LC) and GC were slightly different, despite of the similar homolog composition ratios between the quantification standard and the analytical sample. Although there were discreet discrepancies in the overall chlorine homolog profiles, the carbon chain length profiles acquired from GC and LC were similar. The differences depended on the method employed. Additionally, compared with the low-resolution data, the high-resolution data displayed less fluctuation since the effect of the interferences on the analytical sample was reduced because of the mass accuracy of high-resolution instruments. Accordingly, the interlaboratory trial employing the similar homolog compositional profiles of the quantification standard and the analytical sample proved valuable in elucidating the differences among methods, considering equipment, resolution specification, and ionization.


Asunto(s)
Hidrocarburos Clorados , Parafina , Humanos , Cromatografía de Gases y Espectrometría de Masas/métodos , Parafina/análisis , Cloro/análisis , Hidrocarburos Clorados/análisis , Monitoreo del Ambiente/métodos , Halógenos/análisis , Carbono/análisis , China
6.
Sci Total Environ ; 872: 162187, 2023 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-36781137

RESUMEN

Short-chain chlorinated paraffins (SCCPs) are ubiquitously distributed in various environmental matrics due to their wide production and consumption globally in the past and ongoing production and use in some developing countries. SCCPs have been detected in various human samples including serum, milk, placenta, nail, and hair, and internal SCCP levels were found to be positively correlated with biomarkers of some diseases. While the environmental occurrence has been reported in a lot of studies, the toxicity and underlying molecular mechanisms of SCCPs remain largely unknown. The current tolerable daily intakes (TDIs) recommended by the world health organization/international programme on chemical safety (WHO/IPCS, 100 µg/kg bw/d) and the UK Committee on Toxicity (COT, 30 µg/kg bw/d) were obtained based on a no observed adverse effect level (NOAEL) of SCCP from the repeated-dose study (90 d exposure) in rodents performed nearly 40 years ago. Importantly, the health risks assessment of SCCPs in a variety of studies has shown that the estimated daily intakes (EDIs) may approach and even over the established TDI by UK COT. Furthermore, recent studies revealed that lower doses of SCCPs could also result in damage to multiple organs including the liver, kidney, and thyroid. Long-term effects of SCCPs at environmental-related doses are warranted.


Asunto(s)
Hidrocarburos Clorados , Parafina , Animales , Humanos , China , Cabello/química , Hidrocarburos Clorados/análisis , Leche/química , Parafina/análisis
7.
Sci Total Environ ; 807(Pt 2): 150833, 2022 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-34627908

RESUMEN

Short-chain chlorinated paraffins (SCCPs) are persistent organic pollutants that are present in relatively high concentrations in various environmental media in China. Many studies have focused on chlorinated paraffins in soil from agricultural land and contaminated areas. There are limited data on the levels of chlorinated paraffins in soil from urban areas. In this study, to investigate the levels, distribution, and homolog patterns of chlorinated paraffins (CPs) in soil from a typical urban area, 130 soil samples were collected and combined to form 26 pooled samples. The samples were analyzed for 50 CP congener groups (C9-17Cl5-10). The concentration ranges for SCCPs, medium-chain CPs (MCCP), and chlorinated nonane paraffin (C9-CP) were 19-1456 ng/g (average: 234 ng/g), <10-385 ng/g (average: 54 ng/g), and 1-39 ng/g (average: 11 ng/g), respectively. The CP concentrations were not significantly correlated with the total organic carbon content (P > 0.05). Compared with other areas worldwide, the SCCP and C9-CP concentrations in soil in this area were at the medium level, and the concentrations of MCCPs were at a low level. The CP concentrations were higher in soil samples collected near factories and domestic garbage disposal sites. C10Cl6-7 were the main SCCP homologs and C14Cl7-8 were the main MCCP homologs. Principal component analysis showed that the sources of C9-CPs, SCCPs, and MCCPs in the soils were similar. Risk assessment showed that the concentrations of SCCPs and MCCPs in soil in this area did not pose a significant risk to soil organisms or human health.


Asunto(s)
Parafina , Suelo , China , Humanos
8.
Environ Pollut ; 293: 118456, 2022 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-34740736

RESUMEN

Chlorinated paraffins (CPs) are used as additives in metal processing in the metal smelting industry. Data on CPs in the environment near metal smelting plants are limited. The objectives of this study were to investigate the concentrations and congener profiles of CPs in soil around factories in a non-ferrous metal recycling park located in Hebei, China, and to investigate human exposure to CPs in the soil. The concentrations of short-chain CPs (SCCPs) and medium-chain CPs (MCCPs) were determined by two-dimensional gas chromatography with electron capture negative ionization mass spectrometry. The SCCP and MCCP concentrations in the soil samples were 121-5159 ng/g and 47-6079 ng/g, respectively. Generally, the CP concentrations in soils around the factories were relatively high compared with those near other contaminated sites and in rural and urban areas. There were significant correlations between the MCCP concentrations, some SCCP carbon homologs, and the total organic carbon content (p < 0.05). The major SCCP and MCCP congener groups were C10Cl6-7 and C15-16Cl5, respectively. Hierarchical cluster analysis and principal component analysis indicated that SCCPs and MCCPs in the soil might originate from extreme pressure additives containing CP-42 and CP-52 and CP-containing waste material from the factories. The concentrations in two samples collected near a metal recycling factory posed a moderate risk according to a risk assessment conducted using risk quotients. Further risk assessment showed that the CPs concentrations in soil did not pose significant health risks to either children or adults.


Asunto(s)
Hidrocarburos Clorados , Parafina , Adulto , Niño , China , Monitoreo del Ambiente , Humanos , Hidrocarburos Clorados/análisis , Parafina/análisis , Medición de Riesgo , Suelo
9.
Environ Sci Pollut Res Int ; 29(30): 46273-46281, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35165847

RESUMEN

Chlorinated paraffins are primary industrial chemical products used for metalworking fluids and flame retardants. However, short-chain chlorinated paraffins (SCCPs) are registered in Annex A of the Stockholm Convention on Persistent Organic Pollutants. Therefore, since an accurate quantitative determination of SCCPs is crucial to monitor the level of pollution, analysis quality assurance with reference materials is needed. In this study, a reference material (RM), NMIJ RM 4076-a, was developed by the National Metrology Institute of Japan at the National Institute of Advanced Industrial Science and Technology (NMIJ/AIST) for the quantification of SCCPs. We determined the mass fraction of SCCPs by subtracting the impurities quantified using the mass-balance method, a combination of gas chromatography-flame ionization detection, Karl Fischer titrations, headspace-gas chromatography-mass spectrometry, and thermal gravimetric analysis. The mass fraction value of NMIJ RM 4076-a was concluded to be 0.9996 kg/kg. The standard uncertainty of this mass fraction was evaluated on the basis of the mass-balance method, the sample homogeneity, and stability obtained using the above analytical techniques. Accordingly, the expanded uncertainty estimated using a coverage factor of k = 2 was found to be 0.0013 kg/kg. The mass fraction of chlorine and the homologue compositional ratios are also given for this RM as supplementary technical information. This RM is expected to be applicable for use in the calibration of instruments, or for checking the validity of analytical methods or instruments for estimating the comparability of SCCP analyses.


Asunto(s)
Hidrocarburos Clorados , Parafina , China , Monitoreo del Ambiente/métodos , Ionización de Llama , Cromatografía de Gases y Espectrometría de Masas/métodos , Hidrocarburos Clorados/análisis , Parafina/análisis
10.
Chemosphere ; 279: 130503, 2021 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-33894510

RESUMEN

Dietary intake is an important route of human exposure to chlorinated paraffins (CPs). Cup instant noodles are widely popular food and millions packet of instant noodles are consumed every year. To investigate the levels, congener groups, and health risk of SCCPs and MCCPs in each component of cup instant noodles, samples of nine common brands were collected and analyzed by comprehensive two dimensional gas chromatography coupled with mass spectrometry. The mean concentrations in the noodles were 1.2 × 103 ng/g wet weight (ww) (SCCPs) and 1.2 × 102 ng/g ww (MCCPs), the mean concentrations in the seasoning were 1.4 × 103 ng/g ww (SCCPs) and 1.3 × 102 ng/g ww (MCCPs), and the mean concentrations in the soup were 5.6 × 102 ng/L (SCCPs) and 5.4 × 102 ng/L (MCCPs). The SCCP to MCCP ratio were similar in the soup and soup container, which means CPs in the soup might be migrated from the soup container. Seasoning and noodles from the same brands have similar congener profiles of SCCPs and MCCPs, which may be raised from the manufacturing process or food packaging materials. The dominant SCCP congener groups were C10-11Cl6-7 in noodles and seasoning, and C10,13Cl6-7 in soup. The dominant MCCP congener groups were C14-15Cl6-7 in noodles and seasoning, and C14-15Cl6-7 in soup. A preliminary health risk assessment indicated that the current intakes of SCCPs and MCCPs through cup instant noodles in China did not pose a significant risk to human health.


Asunto(s)
Hidrocarburos Clorados , Parafina , China , Monitoreo del Ambiente , Humanos , Hidrocarburos Clorados/análisis , Parafina/análisis , Medición de Riesgo
11.
Environ Pollut ; 279: 116922, 2021 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-33743436

RESUMEN

Short-chain chlorinated paraffins (SCCPs) are persistent organic pollutants which are toxic to human. Median-chain chlorinated paraffins (MCCPs) have similar toxicity to SCCPs. The productions of chlorinated paraffins (CPs) in China were 1 million tons in 2013 and remained high after that, which may lead to high risks for human exposure to CPs. To investigate temporal trends and health risks of SCCPs and MCCPs in breast milk in China, samples (n = 2020) were collected from urban and rural areas of 11 Chinese provinces in 2017 and mixed into 42 pooled samples. SCCPs and MCCPs were analyzed by two-dimensional gas chromatography with electron-capture negative-ionization mass spectrometry (GC × GC-ECNI-MS). The MCCP concentrations (median (range)) were 472 (94-1714) and 567 (211-1089) ng g-1 lipid in urban and rural areas, respectively, which showed continuously rapidly increasing during 2007-2017. The SCCP concentrations (median (range)) were 393 (131-808) and 525 (139-1543) ng g-1 lipid in urban and rural areas, respectively. The results showed SCCP levels decreased in urban areas between 2007 and 2017. Significant increases in MCCP/SCCP ratios might arise from extensive manufacturing and use of MCCPs. The median estimated dietary intake via breast milk in urban and rural samples were 1230 and 2510 ng kg-1 d-1, respectively, for SCCPs and 2150 and 1890 ng kg-1 d-1, respectively, for MCCPs. Preliminarily risk assessment showed that SCCPs posed a significant health risk to infants via breastfeeding. The high MCCP levels should also be of concern because of continuous growth and negative effect on infants. Correspondence analysis indicated congeners with higher carbon and chlorine numbers in dietary tend to accumulate in breast milk.


Asunto(s)
Hidrocarburos Clorados , Parafina , China , Exposición Dietética , Monitoreo del Ambiente , Femenino , Cromatografía de Gases y Espectrometría de Masas , Humanos , Hidrocarburos Clorados/análisis , Lactante , Leche Humana/química , Parafina/análisis
12.
Sci Total Environ ; 775: 144906, 2021 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-33631584

RESUMEN

In recent years, more attention has been paid to the biological effects of short-chain chlorinated paraffin (SCCP). Studies have shown that SCCPs exposure could cause metabolic damage and lipid metabolic damage. In the present work, based on E. coli membrane damage experiments and molecular dynamics (MD) simulation, the effects of SCCPs on the membrane structure and membrane properties were studied to explore the possible toxic damage effects of SCCPs on cell membrane. Experiments results showed that SCCPs had a significant inhibitory effect on E. coli. The E. coli cell membrane of the bacteria was broken and the macromolecules of the cell flowed out when exposed to SCCPs. SCCPs would lead to the decrease and depolarization of cell membrane potential, and then affect the integrity and permeability of cell membrane. The further molecular dynamic simulation revealed that SCCP molecules can easily enter the lipid DPPC membranes from the aqueous phase and tended to aggregate inside bilayer stably. The bound of SCCPs could lead to significant variations in DPPC bilayer with a less dense, more disorder and rougher layer, which thus made the damage of cell membrane. In a word, although the overall toxicity of SCCPs to cell was relatively weak, the damage to the cell membrane may be one of the mechanisms of its toxicity. MAIN FINDING OF THE WORK: The exposure of SCCPs could cause structural change of cell membrane in E. coli, which verified the damage to the cell membrane may be one of the mechanisms of its toxicity.


Asunto(s)
Hidrocarburos Clorados , Parafina , China , Monitoreo del Ambiente , Escherichia coli , Hidrocarburos Clorados/análisis , Hidrocarburos Clorados/toxicidad , Lípidos , Simulación de Dinámica Molecular , Parafina/análisis , Parafina/toxicidad
13.
Sci Total Environ ; 717: 137204, 2020 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-32065898

RESUMEN

The endangered beluga (Delphinapterus leucas) population residing in the St. Lawrence Estuary (SLE; Eastern Canada) is declining. The elevated tissue concentrations of a wide range of organohalogen contaminants might play a role in the non-recovery of this whale population. Organohalogens have been reported to impair the regulation of several metabolic products from cellular reactions in mammals such as amino acids and fatty acids. The objective of this study was to investigate a suite of organohalogens including polychlorinated biphenyls, organochlorine pesticides, short-chain chlorinated paraffins (SCCPs), polybrominated diphenyl ethers, and selected emerging flame retardants in blubber (biopsy) collected from 40 SLE male belugas, and their relationships to skin concentrations of targeted metabolites (i.e., 21 amino acids, 22 biogenic amines, 18 fatty acids, and 17 energy metabolites). A cluster analysis based on metabolomic profiles distinguished two main subgroups of belugas in the upper and lower sector of their summer habitat in the SLE. These results indicate that ecological factors such as local prey availability and diet composition played a role in shaping the metabolite profiles of belugas. Moreover, SCCP concentrations in SLE male belugas correlated negatively with those of four unsaturated fatty acids (C16:1ω7, C22:5ω3c1, C22:5ω3c2, and C22:6ω3), and positively with those of acetylornithine (biogenic amine). These findings suggest that biological functions such as lipid metabolism represent potential targets for organohalogens in this population, and further our understanding on potential health risks associated with elevated organohalogen exposure in cetaceans. Our results also underscore the necessity of considering ecological factors (e.g., diet and habitat use) in metabolomic studies.


Asunto(s)
Ballena Beluga , Animales , Canadá , Gelatina , Masculino , Bifenilos Policlorados , Contaminantes Químicos del Agua
14.
Chemosphere ; 247: 125855, 2020 May.
Artículo en Inglés | MEDLINE | ID: mdl-31935577

RESUMEN

To preliminarily investigate the occurrence, spatial distributions, homolog compositions, and ecological risks of chlorinated paraffins (CPs) in Yunnan, China, 110 soil samples were collected from an area part of Yunnan, representative of the whole Yunnan area, where had similar characteristics to most parts of Yunnan and 22 pooled soil samples were analyzed for 50 CP congener groups (C9-17Cl5-10). The chlorinated nonane paraffin (C9-CP), short chain (SCCP), and medium chain chlorinated paraffin (MCCP) concentrations in soil samples were 8-109 ng/g (average 39 ng/g), 79-948 ng/g (average 348 ng/g), and 20-1206 ng/g (average 229 ng/g), respectively. The C9-CP homologs contributed 5%-16% of the C9-13-CP concentrations in soils. No significant correlation was found between CP concentrations and the total organic carbon content (P > 0.05). The CP levels in soils from Yunnan were at a medium level compared with those in other areas worldwide. Human activity and atmosphere deposition would influence the levels and spatial distributions of CPs in this area. The concentrations of CPs in east area were higher than those in west area. C10Cl6-7 were the major SCCP congeners and C14Cl6-7 were the major MCCP congeners. Principal component analysis indicated that SCCPs and MCCPs came from different sources. A preliminary risk assessment indicated that these concentrations of CPs in soil from Yunnan do not pose a significant ecological risk for soil organisms.


Asunto(s)
Hidrocarburos Clorados/análisis , Parafina/análisis , Suelo/química , Alcanos/química , China , Monitoreo del Ambiente/métodos , Humanos , Parafina/química , Medición de Riesgo
15.
J Chromatogr A ; 1610: 460550, 2020 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-31547958

RESUMEN

As short-chain chlorinated paraffins (SCCPs) are listed on several monitoring programs, validated methods are essential. However, their complexity and the lack of commercially available certified reference materials (RMs) hinder a proper validation of methods. Instead, one method is usually 'validated' by evaluating performances and results of spiked materials with that of one other method, which could easily lead to unreliable results. This study evaluated four analytical methods with different principles (i.e. comprehensive two dimensional GC coupled to a micro electron capture detector, developed for this study, chloride enhanced atmospheric pressure chemical ionization triple quadrupole time of flight MS (APCI-QToF-HRMS), GC coupled to an electron capture negative ion low resolution MS (GC-ECNI-LRMS) and carbon skeleton GC-MS), investigated the comparability in SCCP determination in spiked and naturally contaminated samples and determined SCCP amounts in candidate RMs for possible certification. The results cast doubt on the use of the most commonly applied method (i.e. GC-ECNI-LRMS), as well as using spiked materials for method validation. The APCI-QToF-HRMS method was found most promising as it achieves the required MS resolution (>21,000), is relatively fast and can detect also other CPs. The suitable identified SCCP levels in the candidate RMs and the agreement in results between the methods bring the first certification of a RM for SCCPs within reach.


Asunto(s)
Contaminantes Ambientales/análisis , Cromatografía de Gases y Espectrometría de Masas/métodos , Cromatografía de Gases y Espectrometría de Masas/normas , Hidrocarburos Clorados/análisis , Parafina/análisis , Monitoreo del Ambiente , Contaminantes Ambientales/química , Hidrocarburos Clorados/química , Parafina/química , Reproducibilidad de los Resultados
16.
J Agric Food Chem ; 68(34): 9043-9051, 2020 Aug 26.
Artículo en Inglés | MEDLINE | ID: mdl-32786846

RESUMEN

Food consumption has been identified as a major pathway for human exposure to short-chain chlorinated paraffins (SCCPs) and medium-chain chlorinated paraffins (MCCPs), but evaluations of SCCP and MCCP intake from major dietary sources are limited. We used the sixth Chinese Total Diet Study to perform a comprehensive investigation of SCCPs and MCCPs in cereals, vegetables, potatoes, legumes, eggs, milk, meats, and aquatic foods from nine southern provinces. The geographical distribution of CP concentrations showed higher levels in Jiangsu, Hubei, and Zhejiang provinces. The CP concentrations in most animal-origin foods were higher than those in foods of plant origin. The total estimated daily intakes (EDIs) of SCCPs and MCCPs, with average values of 7.0 × 102 and 4.7 × 102 ng kg-1 day-1, respectively, were mostly contributed by cereals, vegetables, and meats. Risk assessment indicated the EDIs of CPs posed no significant risk to residents in South China.


Asunto(s)
Contaminación de Alimentos/análisis , Hidrocarburos Clorados/química , Parafina/química , Adolescente , Adulto , Animales , Bovinos , Pollos , China , Exposición Dietética/efectos adversos , Exposición Dietética/análisis , Grano Comestible/química , Grano Comestible/metabolismo , Huevos/análisis , Femenino , Humanos , Hidrocarburos Clorados/metabolismo , Masculino , Carne/análisis , Persona de Mediana Edad , Leche/química , Leche/metabolismo , Parafina/metabolismo , Medición de Riesgo , Alimentos Marinos/análisis , Verduras/química , Verduras/metabolismo , Adulto Joven
17.
Sci Total Environ ; 668: 996-1003, 2019 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-31018478

RESUMEN

Bioaccessibility of short chain chlorinated paraffins (SCCPs), which is important for estimation of dietary exposure, has not been evaluated in previous studies. In the present study, we determined the bioaccessibility of SCCPs in meat (pork, beef and chicken) and seafood (fish, clams, and prawns) using the colon-extended physiologically based extraction test as an in vitro model. The bioaccessibility percentages (BAs) ranged from 33% to 84% in the fed state and from 41% to 63% in the unfed state. The BAs observed in the fed state were lower than in the unfed state in most samples, except for pork sample, which had the highest lipid content. This could be attributed to the effects caused by dietary components added in the fed state. The effects of lipid and protein in samples on bioaccessibility were investigated. In food with a high lipid content, like pork in this study, lipid was the main factor controlling SCCP bioaccessibility. In the other five foods, which had low-medium lipid contents, BA in the unfed state was positively correlated with lipid content (p < 0.05) and negatively correlated with the protein-to-lipid content ratio (p < 0.05). No significant relationships between lipid and protein content and BA were found in the fed state. As to SCCP congener groups, a positive relationship between the BAs of SCCP congener groups and their octanol-water partition coefficients (log Kow) was found in pork sample in the fed state (p < 0.05). The BAs obtained in samples from fish, prawn, clam, and pork in the unfed state and that obtained in clam sample in the fed state were negatively correlated with log Kow (p < 0.05). We calculated more accurate estimated dietary intakes of SCCPs using our SCCP bioaccessibility data. These results will contribute to more reliable dietary risk assessments of SCCPs.


Asunto(s)
Exposición Dietética , Carne , Parafina/análisis , Alimentos Marinos , Contaminación de Alimentos/análisis , Parafina/metabolismo , Medición de Riesgo
18.
Sci Total Environ ; 649: 821-828, 2019 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-30179813

RESUMEN

To investigate the spatial distributions, potential transport and ecological risks of chlorinated paraffins (CPs) in and around e-waste dismantling area, we collected soil samples within 5 km of the e-waste dismantling centers and sediment samples in the surrounding area from the lower reaches of Jiaojiang River. Short- and medium-chain chlorinated paraffins (SCCPs and MCCPs) were analyzed by two-dimensional gas chromatography coupled with electron-capture negative-ionization mass spectrometry (GC × GC-ECNI-MS). The SCCP and MCCP concentration ranges in soils were 68.5 to 2.20 × 105 ng/g dry weight (dw) and 507 to 4.40 × 106 ng/g dw, respectively. The ranges for the levels of SCCPs and MCCPs in sediments were 32.5-1.29 × 104 ng/g dw and 271-2.72 × 104 ng/g dw, respectively. No significant correlation was observed between total organic carbon (TOC) and CP concentrations (P > 0.05). The spatial distributions showed that the CP levels were closely related to e-waste pollution. Correspondence analysis revealed that shorter-chain and less chlorinated congeners were enriched in sediments from sites distant from e-waste pollution source, while longer-chain and higher chlorinated congeners were concentrated in soils and sediments collected near the pollution source, which indicated that complex environmental processes, such as transportation via atmosphere and/or water, and deposition, resulted in different CP profiles in different sampling locations and environment matrixes (e.g., soil and sediments). Principal component analysis (PCA) indicated that e-waste pollution could be the same source of SCCPs and MCCPs. The preliminary risk assessment indicated that CPs in soils within 1 km of e-waste dismantling centers at current levels posed a considerable risk to soil-dwelling organisms, and the sediment MCCPs in Jiaojiang estuary at present levels also posed a risk to sediment-dwelling organisms.

19.
J Hazard Mater ; 380: 120854, 2019 12 15.
Artículo en Inglés | MEDLINE | ID: mdl-31279945

RESUMEN

Short- and medium-chain chlorinated paraffins (SCCPs and MCCPs) in commercial rubber track products and raw materials (rubber granules and adhesives) were investigated by two-dimensional gas chromatography with electron-capture negative-ionization mass spectrometry (GC × GC-ECNI-MS). The mean SCCP and MCCP concentrations in the rubber track products were 3.64 × 103 and 4.14 × 104 µg/g, respectively. The mean SCCP concentration in the products was significantly higher than those in the rubber granules (2.78 µg/g), but in the same order of magnitude as those in the adhesives (3.34 × 103 µg/g). The SCCP concentrations in almost half of the rubber track products and four fifths of the adhesives exceeded the limit (1.5 g/kg) set in Chinese standard GB 36246-2018. The dominant SCCP and MCCP congeners in the rubber track products were similar to those in the relevant adhesives but different from those in the paired granules. Principal component analysis and contribution calculations indicated that chlorinated paraffins (CPs) in adhesives could be the main sources of CPs in rubber track products. The high CP concentrations found in rubber track products are of special concern because of the relatively high exposures for children and negative effect on human health and environment.

20.
J Hazard Mater ; 359: 186-193, 2018 10 05.
Artículo en Inglés | MEDLINE | ID: mdl-30032075

RESUMEN

Short chain chlorinated paraffins (SCCPs) have attracted increasing attention recently due to their widespread occurrence and persistence in the environment, long-distance transport, and bioaccumulation and toxicity. For the sake of photocatalytic elimination of SCCPs, a kind of polydopamine (PDA) based photocatalyst, echinus-like Fe2O3@PDA-Ag hybrids have been synthesized via coating Fe2O3 with PDA by self-polymerization of dopamine and further loading silver nanoparticles by in situ reduction onto the surface of PDA shell. The photogenerated charges of Fe2O3@PDA-Ag hybrids exhibit long lifetime from transient photovoltage signal, which is of benefit to participate in various subsequent reaction processes before their recombination. Benefiting from the coating of PDA shell and the deposition of Ag nanoparticles, Fe2O3@PDA-Ag hybrids exhibit enhanced photocatalytic activity for the removel of SCCPs as investigated by the in situ Fourier transform infrared spectroscopy, 2.9 times as high as that of Fe2O3, due to the reactive OH radicals. The density functional theory simulation demonstrates the key mechanism of the formation of conjugate bond in the dechlorination process as well as the final product of HCl. The simulation indicates that there are no regularities for the H-abstraction but the dechlorination usually occurs in the adjacent Cl atoms next to the C with H-abstraction.

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