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1.
Environ Sci Technol ; 2024 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-39264101

RESUMEN

Incineration is a promising sustainable treatment method for solid waste. However, the ongoing revelation of new toxic pollutants in this process has become a controversial issue impeding its development. Thus, identifying and regulating high-risk pollutants emerge as pivotal strides toward reconciling this debate. In this study, we proposed a workflow aimed at establishing priority monitoring inventories for organic compounds emitted by industries involving full-component structural recognition, environmental behavior prediction, and emission risk assessment, specifically focusing on solid waste incineration (SWI). A total of 174 stack gas samples from 29 incinerators were first collected. Nontarget full organic recognition technology was then deployed to analyze these samples, and 646 organic compounds were identified. The characteristics, i.e., toxicity effects, toxicity concentrations, persistence, and bioaccumulation potential, of these compounds were assessed and ranked based on the TOXCAST database from the US Environmental Protection Agency and structural effect models. Combined with consideration of changes in seasons and waste types, a priority control inventory consisting of 28 organic pollutants was finally proposed. The risks associated with SWI across different regions in China and various countries were assessed, and results pinpointed that by controlling the priority pollutants, the average global emission risk attributed to SWI was anticipated to be reduced by 71.4%. These findings offer significant guidance for decision-making in industrial pollutant management, emphasizing the importance of targeted regulation and monitoring to enhance the sustainability and safety of incineration processes.

2.
Environ Sci Technol ; 57(6): 2217-2234, 2023 02 14.
Artículo en Inglés | MEDLINE | ID: mdl-36722466

RESUMEN

Understanding the mechanisms through which persistent organic pollutants (POPs) form during combustion processes is critical for controlling emissions of POPs, but the mechanisms through which most POPs form are poorly understood. Polyhalogenated dibenzo-p-dioxins and dibenzofurans (PXDD/Fs) are typical toxic POPs, and the formation mechanisms of PXDD/Fs are better understood than the mechanisms through which other POPs form. In this study, a framework for identifying detailed PXDD/Fs formation mechanisms was developed and reviewed. The latest laboratory studies in which organic free radical intermediates of PXDD/Fs have been detected in situ and isotope labeling methods have been used to trace transformation pathways were reviewed. These studies provided direct evidence for PXDD/Fs formation pathways. Quantum chemical calculations were performed to determine the rationality of proposed PXDD/Fs formation pathways involving different elementary reactions. Many field studies have been performed, and the PXDD/Fs congener patterns found were compared with PXDD/Fs congener patterns obtained in laboratory simulation studies and theoretical studies to mutually verify the dominant PXDD/Fs formation mechanisms. The integrated method involving laboratory simulation studies, theoretical calculations, and field studies described and reviewed here can be used to clarify the mechanisms involved in PXDD/Fs formation. This review brings together information about PXDD/Fs formation mechanisms and provides a methodological framework for investigating PXDD/Fs and other POPs formation mechanisms during combustion processes, which will help in the development of strategies for controlling POPs emissions.


Asunto(s)
Dioxinas , Contaminantes Ambientales , Dibenzofuranos , Contaminantes Ambientales/análisis , Dibenzofuranos Policlorados
3.
Environ Sci Technol ; 57(4): 1646-1657, 2023 01 31.
Artículo en Inglés | MEDLINE | ID: mdl-36681930

RESUMEN

Chlorinated organic chemicals are produced and used extensively worldwide, and their risks to the biology and environment are of increasing concern. However, chlorinated byproducts [e.g., polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs)] formed during the commercial manufacturing processes and present in organochlorine products are rarely reported. The knowledge on the occurrences and fate of unintentional persistent organic chemicals in the manufacturing of organochlorine chemical is necessary for accurate assessment of the risks of commercial chemicals and their production. Here, PCDD/Fs were tracked throughout chlorobenzene and chloroethylene production processes (from raw materials to final products) by target analysis. Other byproducts that can further transform into PCDD/Fs were also identified by performing non-target screening. As a result, the PCDD/F concentrations were mostly the highest in bottom residues, and the octachlorinated congeners were dominant. Alkali/water washing stages may cause the formation of oxygen-containing byproducts including PCDD/Fs and acyl-containing compounds, so more attention should be paid to these stages. PCDD/Fs were of 0.17 and 0.21-1.2 ng/mL in monochlorobenzene and chloroethylene products, respectively. Annual PCDD/F emissions (17 g toxic equivalent in 2018) during chlorobenzene and chloroethylene production were estimated using PCDD/F emission factors. The results can contribute to the improvement of PCDD/F inventories for the analyzed commercial chemicals.


Asunto(s)
Dibenzodioxinas Policloradas , Cloruro de Vinilo , Dibenzofuranos/análisis , Cloruro de Vinilo/análisis , Dibenzofuranos Policlorados/análisis , Dibenzofuranos Policlorados/química , Monitoreo del Ambiente , Clorobencenos
4.
Rapid Commun Mass Spectrom ; 36(14): e9324, 2022 Jul 30.
Artículo en Inglés | MEDLINE | ID: mdl-35560965

RESUMEN

RATIONALE: Polyhalogenated carbazoles (PHCZs) are dioxin-like compounds that are ubiquitous in the environment. However, their unintentional emissions from industrial sources have received little attention and there is no method available for determination of PHCZs in industrial waste. This research develops a method for determination of PHCZs in industrial waste. METHODS: In this research, a glass column packed with activated silica serves as a rapid and efficient clean-up pretreatment for purification. An isotope dilution gas chromatography/triple quadrupole tandem mass spectrometry method was established for simultaneous determination of eleven PHCZs in industrial samples. RESULTS: The regression coefficients of the standard curves for the congeners were all >0.99. The method detection limit ranged from 1.46 to 3.82 ng/mL for liquid samples and from 0.009 to 0.021 ng/g for solid samples. The precision described by the relative standard deviation ranged from 2.4% to 18.4% for liquid samples and from 5.5% to 35.8% for solid samples. The recovery ranges for the liquid and solid samples were 82%-123% and 83%-137%, respectively. 3-Chlorocarbazole (3-CCZ) and 36-dichlorocarbazole (36-CCZ) can be detected in both chemical bottom liquid from vinyl chloride production and fly ash from medical waste incineration by this method. CONCLUSIONS: An efficient method is established for determination of PHCZs from industrial waste. The discovery of 3-CCZ and 36-CCZ highlights the importance of identification of potential industrial sources of PHCZs and clarification of their contribution to environmental risks. Our method could be applied to investigate industrial emission of PHCZs.


Asunto(s)
Residuos Industriales , Espectrometría de Masas en Tándem , Carbazoles/análisis , Carbazoles/química , Cromatografía de Gases y Espectrometría de Masas , Residuos Industriales/análisis
5.
Environ Sci Technol ; 56(20): 14550-14561, 2022 10 18.
Artículo en Inglés | MEDLINE | ID: mdl-36168137

RESUMEN

Metal compounds play important roles in the formation of organic pollutants during thermal-related processes. However, the metal-catalyzed predominant organic pollutants have not previously been characterized nor have any detailed catalytic mechanisms been clarified. Here, we preciously distinguished the multiple organic free radical intermediates on metal catalyst surfaces during the organic pollutant formation through laboratory and theoretical studies. Differences between the organic free radical intermediate species, concentrations, and formation mechanisms under the catalysis of different metal compounds were investigated. The results were verified mutually with the differed characteristics of organic pollutant products. CuO predominantly catalyzed the formation of highly chlorinated phenoxy radical intermediates and dioxins. High proportions of semiquinone radicals and oxygen-containing derivatives were found on ZnO surfaces. Differently, methyl-substituted phenoxy radicals and long-chain products formed on Al2O3 surfaces. The results will be instructive for the target emission control of priority organic pollutants during thermal-related processes rich in different metal compounds.


Asunto(s)
Dioxinas , Contaminantes Ambientales , Óxido de Zinc , Catálisis , Radicales Libres , Metales , Oxígeno
6.
Environ Sci Technol ; 56(9): 5520-5529, 2022 05 03.
Artículo en Inglés | MEDLINE | ID: mdl-35417140

RESUMEN

Intake from food is considered an important route of human exposure to polychlorinated naphthalenes. To our knowledge, several studies have quantified dietary exposure but only in European countries and measuring only a few of the 75 congeners. In addition, the influence of source diversity on human exposure has seldom been assessed. We analyzed 192 composite food samples composed of 17,280 subsamples from 24 provinces in China to measure the concentrations of polychlorinated naphthalenes and estimate their daily intake and potential health risks on a national scale. The estimated cancer risk was in the range of 6.8 × 10-8 to 4.6 × 10-7. We compared our findings for 75 congeners with reports in the literature that quantified only 12 congeners. We estimate that these 12 congeners contribute only approximately 4% to the total mass daily intake of polychlorinated naphthalenes and 70% to the total toxic equivalent quantity, indicating underestimation of dietary exposure. The contributions of combustion-associated congeners to the total concentrations of polychlorinated naphthalenes were in the range of 31-52%, suggesting that the ongoing unintentional release of these compounds from industrial thermal processes is an important factor in polychlorinated naphthalene contamination and human exposure in China.


Asunto(s)
Exposición Dietética , Bifenilos Policlorados , China , Dibenzofuranos Policlorados , Monitoreo del Ambiente , Humanos , Industrias , Naftalenos/toxicidad
7.
J Clin Lab Anal ; 36(4): e24306, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35195921

RESUMEN

OBJECTIVE: Detecting neutralizing antibodies targeting receptor-binding domain (RBD) is important for the assessment of humoral protection and vaccine efficacy after vaccination. We compared the performance of three surrogate immunoassays for detection of neutralizing antibodies targeting RBD. METHODS: We analyzed 115 serum samples obtained from individuals with Ad5-vectored COVID-19 vaccination using two competitive enzyme-linked immunosorbent assays (Wantai BioPharm and Synthgene Medical Technology) and one competitive chemiluminescence assay (YHLO Biotech). Performance evaluation and methodology comparison were performed according to the Clinical and Laboratory Standards Institute related guidelines. RESULTS: The precision met the manufacturers' statements. The linear range of the WANTAI was 0.0625-0.545 U/ml and the YHLO was 0.260-242.4 U/ml. The WANTAI's limit of blank (LoB) and limit of detection (LoD) were 0.03 and 0.06 U/ml, respectively. The YHLO's LoB and LoD were 0.048 and 0.211 U/ml, respectively. The correlations of semi-quantitative results of Synthgene with quantitative results of YHLO (ρ = 0.566) and WANTAI (ρ = 0.512) were medium. For YHLO and WANTAI, there was a good agreement (0.62) and a strong correlation (ρ = 0.931). Passing-Bablok analysis and Bland-Altman plot showed a positive bias (112.3%) of the YHLO compared to the WANTAI. The exclusion of samples >50 U/ml did not decrease bias. CONCLUSION: These findings contribute to a deeper understanding of surrogate viral neutralization assays and provide useful data for future comparison studies.


Asunto(s)
COVID-19 , SARS-CoV-2 , Adenoviridae/genética , Anticuerpos Neutralizantes , Anticuerpos Antivirales , Vacunas contra la COVID-19 , Humanos , Inmunoensayo/métodos , Vacunación
8.
Ecotoxicol Environ Saf ; 238: 113594, 2022 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-35525118

RESUMEN

Chlorinated and brominated polycyclic aromatic hydrocarbons (Cl/Br-PAHs) are emerging persistent organic pollutants. Current knowledge on the emissions of Cl/Br- PAHs is far insufficient for source control, much less on their formation mechanisms. In this field study, Cl/Br-PAHs formation mechanisms were proposed from the macro perspective of practical secondary metal smelting industries. We found secondary zinc smelting as a significant source of Cl/Br-PAHs (9553 ng/m3 in stack gas), exceeding concentrations from other metal smelting sources by 1-2 orders of magnitude. Cl/Br-PAH emission characteristics differed between various secondary metal smelting processes, indicating dominance of different formation mechanisms. Cl/Br-PAHs with fewer rings were dominant from secondary zinc smelting and secondary copper smelting. Differently, emissions from secondary aluminum smelting were dominated by congeners with more rings. The differences in congener profiles were attributable to the catalytic effects of metal compounds during smelting activities. Zinc oxide and copper oxide dominantly catalyzed dehydrogenation reactions, contributing to the formation of intermediate radicals and subsequent dimerization to Cl/Br-PAHs with fewer rings. Differently, aluminum oxide induced alkylation reactions and accelerated ring growth, resulting in the formation of Cl-PAHs with more rings. The newly proposed mechanisms can successfully explain the emission characteristics of Cl/Br-PAHs during smelting activities, which should be important implication for Cl/Br-PAHs targeted source control.


Asunto(s)
Contaminantes Atmosféricos , Hidrocarburos Clorados , Hidrocarburos Policíclicos Aromáticos , Contaminantes Atmosféricos/análisis , Cobre , Monitoreo del Ambiente , Hidrocarburos Clorados/análisis , Hidrocarburos Policíclicos Aromáticos/análisis , Zinc
9.
J Environ Sci (China) ; 121: 159-174, 2022 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-35654507

RESUMEN

In this study, concentrations of Cr, Mn, Ni, Cu, Zn, Cd and Pb were determined in road dusts collected from different locations in Dhaka to assess source, contamination status and health risk. Energy-dispersive X-ray fluorescence spectroscopy and energy-dispersive X-ray spectroscopy were used to determine Cr, Mn, Ni, Cu, Zn, Cd and Pb and their mean concentrations were 162.27 ± 29.46, 721.18 ± 180.14, 35.65 ± 12.55, 104.56 ± 128.33, 515.32 ± 321.90, BDL, and 342.82 ± 591.20 mg/kg, respectively. Among the heavy metals, highest concentrations of Cu, Zn and Pb were found at urban sites-7 (municipal waste dumping) and 8 (medical waste incineration). Highest concentration of Cr followed by Cu and Zn was found at site-5 (Tejgaon, urban). Principal component analysis revealed that anthropogenic activities are the potential sources for Cr, Ni, Cu, Zn and Pb while earth crust for Mn. Pollution index and pollution load index results suggested that all the sites were contaminated and/or degraded by Cr, Cu, Zn and Pb except sites-9 (urban), 10 (sub-urban), 11 (rural) while sites-7 and 8 (urban) were extremely degraded. For noncarcinogenic health risk, hazard quotient values for dermal were higher compared to that of inhalation/ingestion. Though hazard index values were less than 1 at all the sites, these were at least one order of magnitude higher for children group than that of adult group, thus the children group may face more noncarcinogenic health risk at sites-7 and 8. Values of incremental lifetime cancer risk were from 10-9 to 10-11 showed no carcinogenic health risk by road dusts contaminated with the heavy metals.


Asunto(s)
Polvo , Metales Pesados , Adulto , Bangladesh , Cadmio/análisis , Niño , Polvo/análisis , Monitoreo del Ambiente/métodos , Humanos , Plomo/análisis , Metales Pesados/análisis , Medición de Riesgo
10.
Environ Sci Technol ; 55(10): 6529-6541, 2021 05 18.
Artículo en Inglés | MEDLINE | ID: mdl-33956443

RESUMEN

Attention is increasingly being paid to environmentally persistent free radicals (EPFRs), which are organic pollutants with the activities of free radicals and stabilities of organic pollutants. EPFRs readily form during thermal processes through the decomposition of organic precursors such as phenols, halogenated phenols, and quinone-type molecules, which are also important precursors of toxic unintentionally produced persistent organic pollutants (UPOPs). We have found that EPFRs are important intermediates for UPOP formation during thermal-related processes. However, interest in EPFRs is currently mostly focused on the toxicities and formation mechanisms of EPFRs themselves. Little information is available on the important roles EPFRs play in toxic UPOP formation during thermal processes. Here, we review the mechanisms involved in EPFR formation and transformation into UPOPs during thermal processes. The review is focused on typical EPFRs, including cyclopentadiene, phenoxy, and semiquinone radicals. The reaction temperature, metal species present, and oxygen concentration strongly affect EPFR and UPOP formation during thermal-related processes. Gaps in current knowledge and future directions for research into EPFR and UPOP formation, transformation, and control are presented. Understanding the relationships between EPFRs and UPOPs will allow synergistic control strategies to be developed for thermal-related industrial sources of EPFRs and UPOPs.


Asunto(s)
Contaminantes Ambientales , Material Particulado , Radicales Libres/análisis , Metales , Material Particulado/análisis , Contaminantes Orgánicos Persistentes
11.
Environ Sci Technol ; 55(23): 15929-15939, 2021 12 07.
Artículo en Inglés | MEDLINE | ID: mdl-34812043

RESUMEN

Chlorinated polycyclic aromatic hydrocarbons including chlorinated naphthalenes and congeners with three to five rings are ubiquitous atmospheric pollutants. Congener profiles and formation mechanisms from typical chemical manufacturing have not been researched extensively. We measured the concentrations of 75 chlorinated naphthalenes and 18 chlorinated polycyclic aromatic hydrocarbons in raw materials, intermediates, products, and bottom residues from chemical plants producing monochlorobenzene and chloroethylene by different techniques. The findings confirmed that these chemical manufacturing processes are newly identified sources of atmospheric emissions of these compounds. More-chlorinated naphthalenes were formed from chloroethylene production than from monochlorobenzene production, which could be explained by the higher temperatures in the former process. Successive chlorination appeared to be an important formation pathway of polychlorinated naphthalenes according to their congener profiles and was supported by quantum chemical calculations of electrophilic chlorination on various positions of naphthalene. Chlorinated polycyclic aromatic hydrocarbons were more likely to be formed during the production of monochlorobenzene than chloroethylene. Moreover, we suggested that ring rearrangement and ring coupling are important transformation reactions between polychlorinated naphthalenes and chlorinated polycyclic aromatic hydrocarbons.


Asunto(s)
Hidrocarburos Clorados , Hidrocarburos Policíclicos Aromáticos , Cloruro de Vinilo , Clorobencenos , Monitoreo del Ambiente , Hidrocarburos Clorados/análisis , Hidrocarburos Policíclicos Aromáticos/análisis
12.
Environ Sci Technol ; 55(10): 6804-6813, 2021 05 18.
Artículo en Inglés | MEDLINE | ID: mdl-33929821

RESUMEN

Polychlorinated naphthalenes (PCNs) are carcinogenic contaminants. Residues from historical production and ongoing unintentional releases from industrial thermal sources have led to the ubiquitous presence of PCNs in the environment. Our previous study has revealed that unintentional releases may be the main sources of PCNs in human milk from China. However, an assessment of PCN burden in human milk and exposure differences between historical residues and unintentional release exposure has not been conducted. In this study, we performed the first comparison of human exposure to PCNs and evaluated the differences between the estimated health risks from historical residues and unintentional releases. Three characteristic PCN congener patterns found in Chinese human milk specimens collected from 100 cities/counties can be considered characteristic of PCN exposures in regions with unintentional industrial releases as the main PCN sources. The health risk assessment suggested potential noncarcinogenic health effects in infants aged 0-6 months. The hazard index calculated for infants in Sweden indicates a strong impact of historical residues that nonetheless decreases over time, and a comparison of the hazard indices calculated for China and Ireland suggests that ongoing unintentional formation and release of PCNs from industrial processes should be a matter of public health concern.


Asunto(s)
Leche Humana , Naftalenos , China , Ciudades , Monitoreo del Ambiente , Humanos , Lactante , Irlanda , Leche Humana/química , Naftalenos/análisis , Suecia
13.
BMC Infect Dis ; 21(1): 127, 2021 Jan 29.
Artículo en Inglés | MEDLINE | ID: mdl-33514323

RESUMEN

BACKGROUND: To investigate the CT imaging and clinical features of three atypical presentations of coronavirus disease 2019 (COVID-19), namely (1) asymptomatic, (2) CT imaging-negative, and (3) re-detectable positive (RP), during all disease stages. METHODS: A consecutive cohort of 79 COVID-19 patients was retrospectively recruited from five independent institutions. For each presentation type, all patients were classified into atypical vs. typical groups (i.e., asymptomatic vs.symptomatic, CT imaging-negative vs. CT imaging-positive, and RP and non-RP,respectively). The chi-square test, Student's t test, and Kruskal-Wallis H test were performed to compare CT imaging and clinical features of atypical vs. typical patients for all three presentation categories. RESULTS: In our COVID-19 cohort, we found 12.7% asymptomatic patients, 13.9% CT imaging-negative patients, and 8.9% RP patients. The asymptomatic patients had fewer hospitalization days (P=0.043), lower total scores for bilateral lung involvement (P< 0.001), and fewer ground-glass opacities (GGOs) in the peripheral area (P< 0.001) than symptomatic patients. The CT imaging-negative patients were younger (P=0.002), had a higher lymphocyte count (P=0.038), had a higher lymphocyte rate (P=0.008), and had more asymptomatic infections (P=0.002) than the CT imaging-positive patients. The RP patients with moderate COVID-19 had lower total scores of for bilateral lung involvement (P=0.030) and a smaller portion of the left lung affected (P=0.024) than non-RP patients. Compared to their first hospitalization, RP patients had a shorter hospitalization period (P< 0.001) and fewer days from the onset of illness to last RNA negative conversion (P< 0.001) at readmission. CONCLUSIONS: Significant CT imaging and clinical feature differences were found between atypical and typical COVID-19 patients for all three atypical presentation categories investigated in this study, which may help provide complementary information for the effective management of COVID-19.


Asunto(s)
COVID-19/diagnóstico por imagen , Pulmón/diagnóstico por imagen , Radiografía Torácica , Tomografía Computarizada por Rayos X , Adulto , Infecciones Asintomáticas , COVID-19/epidemiología , China/epidemiología , Femenino , Hospitalización , Humanos , Masculino , Persona de Mediana Edad , Readmisión del Paciente , Estudios Retrospectivos , SARS-CoV-2
14.
J Clin Lab Anal ; 35(6): e23788, 2021 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-33955043

RESUMEN

BACKGROUND: Circular RNAs (circRNAs) are involved in various diseases and serve as biomarkers. The present study aimed to investigate unique expression profiles of circRNAs in colon tissues of Crohn's disease (CD) and search novel biomarkers for the diagnosis. METHODS: Differentially expressed (DE) circRNAs in biopsies from four CD patients, four ulcerative colitis (UC) patients, and four healthy controls (HC) were screened by microarray. Hsa_circ_0062142 and hsa_circ_0001666 were verified in another expanded validation cohort. Bioinformatics analysis was applied to predict the function of two DE circRNAs. Receiver operating characteristic (ROC) curves were constructed to evaluate the diagnostic value of CD. RESULTS: The top 10 upregulated circRNAs in CD compared with HC were hsa_circ_0000691, hsa_circ_0001666, hsa_circ_0004183, hsa_circ_0009024, hsa_circ RNA_405324, hsa_circ_0002003, hsa_circ_0085323, hsa_circ_0040994, hsa_circ_0062142, and hsa_circ_0048148; the top 10 downregulated circRNAs were hsa_circ_0049356, hsa_circ RNA_405443, hsa_circ RNA_403556, hsa_circ_0092328, hsa_circ_0003979, hsa_circ_0074491, hsa_circ_0023461, hsa_circ RNA_406237, hsa_circ_0034044, and hsa_circ RNA_400564 (fold change in descending order). The expression levels of hsa_circ_0001666 and hsa_circ_0062142 in CD were significantly higher than those in UC and HC (p < 0.01). ROC curves suggested the favorable diagnostic value of hsa_circ_0062142 and hsa_circ_0001666 (AUC = 0.803 and 0.858, respectively, p < 0.01). In silico analysis indicated that these circRNAs may be involved in the progress of CD. CONCLUSION: Hsa_circ_0062142 and hsa_circ_0001666 may play critical roles in the pathogenesis and serve as potential biomarkers of CD.


Asunto(s)
Biomarcadores/metabolismo , Colon/metabolismo , Biología Computacional/métodos , Enfermedad de Crohn/patología , Análisis por Micromatrices/métodos , ARN Circular/genética , Biomarcadores/análisis , Estudios de Casos y Controles , Estudios de Cohortes , Enfermedad de Crohn/genética , Enfermedad de Crohn/cirugía , Estudios de Seguimiento , Humanos , Pronóstico
15.
Ecotoxicol Environ Saf ; 208: 111722, 2021 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-33396053

RESUMEN

The amount of steel produced using electric arc furnaces (EAFs) has been increasing in recent years. In this study, stack gases from EAFs in steelmaking plants were analyzed to determine if they are also dominant sources of polybrominated dibenzo-p-dioxin and dibenzofuran (PBDD/F) emissions in China. Isotope dilution high-resolution gas chromatography high-resolution mass spectrometry for qualitative and quantitative analysis of PBDD/F congeners revealed that the mean PBDD/F mass concentrations were 271.1-9467.8 pg Nm-3 for the preheating stages (PS) of three EAF plants and that the corresponding toxic equivalents (TEQs) were 10.8-971.2 pg TEQ Nm-3. The PBDD/F mass concentration from the smelting stage (SS) at plant E3 was 261.9 pg Nm-3 (4.5 pg TEQ Nm-3). The PBDD/F emission factors (EF) during the preheating stage for the three plants were 0.0356-1.51 µg TEQ t-1, and the EF was 0.0359 µg TEQ t-1 during the E3 smelting stage. PBDD/Fs were found to contribute 2.39-67.85% to the total mass and 2.84-57.68% to the total dioxin TEQ. These wide fluctuations were caused by differences in the composition of feeding materials and the working temperature of bag filters. Overall, the results indicate that PBDD/F emissions from EAF steelmaking should receive increased attention. The PBDD/F congener patterns among the three EAF plants were variable, possibly because of differences in raw materials. The results presented herein will facilitate assessment of the contribution of EAFs to total PBDD/F emissions in China and investigations of PBDD/F emissions at different stages of steelmaking processes using EAFs.


Asunto(s)
Contaminantes Atmosféricos/análisis , Dibenzofuranos/análisis , Dioxinas/análisis , Metalurgia , Emisiones de Vehículos/análisis , China , Electricidad , Monitoreo del Ambiente , Gases/análisis , Metalurgia/instrumentación , Acero
16.
Bull Environ Contam Toxicol ; 106(4): 670-675, 2021 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-33486542

RESUMEN

Electric arc furnaces (EAFs) in steelmaking plants are a major source of dioxins. Preheating of steelmaking raw materials is widely used in EAFs to reduce energy consumption. Few studies have investigated emissions of dioxin-like polychlorinated biphenyls (PCBs) from EAFs, and the PCB emission levels and characteristics during preheating are unknown. In this study, PCB concentrations and distributions in stack gases emitted during EAF preheating were determined. The average dioxin-like PCB concentrations in stack gases emitted during preheating of three EAFs were 1236.1, 81,664.4, and 669.8 pg/Nm3, respectively. These values were greatly influenced by the composition of the steelmaking raw materials. The PCB profiles in all samples were dominated by less-chlorinated homologs. PCB emission factor for preheating in the EAFs is 0.58 µg WHO-TEQ/ton averagely, indicating significant emissions of PCBs from preheating process. The data will be useful for developing approaches for preventing and controlling PCB emissions from EAFs.


Asunto(s)
Dioxinas , Bifenilos Policlorados , Dibenzodioxinas Policloradas , Dibenzofuranos Policlorados , Dioxinas/análisis , Monitoreo del Ambiente , Gases/análisis , Bifenilos Policlorados/análisis , Dibenzodioxinas Policloradas/análisis
17.
Small ; 16(47): e2001377, 2020 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-33140550

RESUMEN

In this work, an L-shaped silver complex, AgLClO4 (L = 2,3-bis[3-(pyridin-2-yl)-1H-pyrazol-1-yl·methyl]quinoxaline), M, is found to be adaptable enough to host a range of medium and large aromatic hydrocarbons including several polycyclic aromatic hydrocarbons (PAHs). The transformation of M from as-synthesized closed (nonporous) crystalline to at least three types of open phase structures in the presence of different aromatic hydrocarbons enables the adaptable binding of M to these aromatics. In essence, M can rearrange its cavities to fit the different sizes and shapes of the guest molecules in the manner that is infeasible with cage compounds or coordination networks. Single-crystal and powder X-ray diffraction confirm the adaptable structures of the resulting host-guest complexes, M·nG (G = guest, n = 0.5 or 0.75). Detailed 1D and 2D nuclear magnetic resonance spectra, along with the fluorescence spectroscopy, reveal that the host-guest complexes feature similar chemical compositions in the solution, but are in the states of rapid exchange in and outside the cages. Such an adaptability of M provides insights into the strength of host-guest interactions and enables a new class of adsorptive molecular materials that can bind a large number of aromatics, specifically PAHs.

18.
Chem Res Toxicol ; 33(9): 2446-2454, 2020 09 21.
Artículo en Inglés | MEDLINE | ID: mdl-32786545

RESUMEN

Balkan endemic nephropathy (BEN) is a slowly progressive interstitial fibrotic disease affecting numerous people living along the Danube River in the Balkan Peninsula, of which aristolochic acids (AAs) produced naturally in Aristolochia plants are key etiological agents. However, the exposure biology of the disease remains poorly understood. Initially, the high incidence of BEN in the Balkan Peninsula was thought to occur through ingestion of bread prepared from flour made with wheat grains comingled with the seeds of Aristolochia clematitis L., an AA-containing weed that grows abundantly in the wheat fields of the affected areas. In this study, by a liquid chromatography-tandem mass spectrometry (LC-MS/MS) method, we show for the first time that vegetables, in particular root vegetables of endemic areas, are extensively contaminated with AAs taken up through root absorption from the AA-tainted soil. Furthermore, we found a pH dependence of the n-octanol/water partition coefficient (Kow) of AAs, which resulted in a dramatically higher hydrophobicity-driven plant uptake efficiency of AAs into food crops in endemic areas, characterized by higher acidity levels, compared to non-endemic areas. We believe the results of this study have significantly unraveled the mystery surrounding the uneven distribution of BEN incidence.


Asunto(s)
Ácidos Aristolóquicos/efectos adversos , Ácidos Aristolóquicos/análisis , Nefropatía de los Balcanes/inducido químicamente , Contaminantes Ambientales/efectos adversos , Contaminantes Ambientales/análisis , Contaminación de Alimentos/análisis , Aristolochia/química , Cromatografía Líquida de Alta Presión , Abastecimiento de Alimentos , Humanos , Concentración de Iones de Hidrógeno , Estructura Molecular , Semillas/química , Espectrometría de Masas en Tándem , Verduras/química
19.
Environ Sci Technol ; 54(2): 842-850, 2020 01 21.
Artículo en Inglés | MEDLINE | ID: mdl-31859492

RESUMEN

Polychlorinated naphthalenes (PCNs) are highly toxic persistent organic pollutants (POPs) that are a relatively new addition to the Stockholm Convention as of 2015. The levels of unintentional emissions of PCNs from important industrial thermal sources on national scales are unclear but are important for understanding potential human exposure. In this study, an inventory was compiled of PCN emissions from priority industrial sources of unintentional POPs in China. Estimated emissions from four typical POP sources in the reference year (2014) in China were 511.6 kg by mass and 7650.8 mg of toxic equivalent. Waste incineration, secondary nonferrous smelting, electric arc furnace steelmaking, and iron ore sintering plants contributed 38.8, 15.4, 29.2, and 16.6%, respectively, to the total emissions. The Eastern Seaboard of China and the Hebei region in North China, which have intensive industrial activity and high population densities, were dominant contributors of PCNs. Only 18.6% of the counties where waste incineration plants were located emitted PCNs at a level higher than 1.00 × 10-1 mg of toxic equivalent, whereas 80% of the counties where metallurgical plants were located emitted PCNs at this level. These results indicate effective implementation of POP control in the waste incineration industry in China. This study clarifies the unintentionally emission levels of PCNs in China and provides important information for strategy development to control source emissions.


Asunto(s)
Contaminantes Atmosféricos , Incineración , China , Dibenzofuranos Policlorados , Monitoreo del Ambiente , Metalurgia , Naftalenos
20.
Environ Sci Technol ; 54(4): 2314-2322, 2020 02 18.
Artículo en Inglés | MEDLINE | ID: mdl-31951122

RESUMEN

Polychlorinated naphthalenes (PCNs) are globally transported, carcinogenic, persistent organic pollutants (POPs) that were recently added to the Stockholm Convention with 184 parties. The Tibetan Plateau plays an important role in the global transportation and distribution of POPs. Knowledge of PCN sources and transportation on the Tibetan Plateau is important for their control globally. In this study, we quantified the congener-specific concentrations of PCNs in lichen, moss, soil, and air samples collected on the Tibetan plateau and found that common lichens were effective biomonitors for predicting atmospheric PCNs in this area. The physiochemical properties of the PCNs, the temperatures, and the lichen lipid contents were identified as important factors influencing PCN partitioning between lichens and air. Lichen-air partitioning equations were established and used to predict PCN concentrations in air in Southeast Tibet. The lichens could be used as PCN biomonitors to clarify their spatial variations, sources, and transportation in the southeast of the plateau. PCN concentrations in lichens increased with altitude, suggesting that high-mountain cold-trapping influenced the PCN transportation behavior. Principal component analysis and linear discriminant analysis showed that the major source of PCNs in this region was long-range atmospheric transportation via the Indian monsoon in summer and wind from Southwest Asia in winter. This study provides a novel method using PCN congener profiles as fingerprints and statistical models for studying the geochemical effects of conditions in high-mountain regions on the contamination behaviors of 75 congeners of the notorious PCNs.


Asunto(s)
Contaminantes Atmosféricos , Hidrocarburos Clorados , Líquenes , Monitoreo del Ambiente , Naftalenos , Suelo , Tibet
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