The research progress on the mechanisms of formation and degradation of polychlorinated dibenzo-p-dioxins ( PCDDs ) and dibenzofurans ( PCDFs ) is reviewed. The primary sources of PCDD/Fs are chemical, thermal, photoc...The research progress on the mechanisms of formation and degradation of polychlorinated dibenzo-p-dioxins ( PCDDs ) and dibenzofurans ( PCDFs ) is reviewed. The primary sources of PCDD/Fs are chemical, thermal, photochemical and enzymatic reactions. Most of the thermal sources result in emissions into air. The studies on the photodegradation and biodegradation offer promise for destruction of PCDD/Fs in environment.展开更多
We analyzed polychlorinated dibenzofurans (PCDF) and dibenzo-p-dioxins (PCDD) in 27 tree bark samples from the industrialized area near Sauget, Illinois, USA. The trees were located within 4 km of the W. G. Krummrich ...We analyzed polychlorinated dibenzofurans (PCDF) and dibenzo-p-dioxins (PCDD) in 27 tree bark samples from the industrialized area near Sauget, Illinois, USA. The trees were located within 4 km of the W. G. Krummrich (WGK) plant, the oldest and largest chemical plant in Sauget, with 24 of 27 samples collected from residential areas. The percent of total PCDF or PCDD profiles of ten 2,3,7,8- Cl substituted PCDF and seven PCDD congeners is homogeneous: 90% of the variance among the samples is explained by 3 eigenvalues in a principal components analysis. The homogeneity of the data suggests that samples were affected by similar types of sources which may have been influenced by electric power generation, chemical waste incineration, and large-scale thermal production of chlorinated chemicals. Quantitatively, the 2,3,7,8-Cl substituted congener analysis does not account for 90% of the concentration of tetra- and penta-Cl homologues and 80% of hexa-Cl and 50% of hepta-Cl homologues. The World Health Organization stated during establishment of toxic equivalence factors (TEF, 2005 version) that calculation of toxic equivalents (TEQs) is not suitable for abiotic matrices, such as tree bark, which are not involved in human exposures. Our results show that the non-2,3,7,8-Cl substituted congeners have high concentrations and should be included in analysis.展开更多
Labeled polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)were extracted by three different methods,i.e.,soxhlet extraction,hot extraction and accelerated solvent extraction(ASE).The PCDD/Fs were detected by...Labeled polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)were extracted by three different methods,i.e.,soxhlet extraction,hot extraction and accelerated solvent extraction(ASE).The PCDD/Fs were detected by high resolution gas chromatography-high resolution mass spectrometry.Comparisons of the three methods were carried out by recovery of PCDD/Fs,solvent consumption and extraction time.The results showed that all of the method could extract labeled PCDD/Fs efficiently.ASE was a time saving procedure with lowest consumption of solvents compared with the other two methods.展开更多
A rapid pretreatment method of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in soil and analysis by high resolution gas chromatograph-high resolution mass spectrometry was present.The extraction and a...A rapid pretreatment method of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in soil and analysis by high resolution gas chromatograph-high resolution mass spectrometry was present.The extraction and alumina clean up of PCDD/Fs in soil was achieved by accelerated solvent extractor.Then the multi-layer silica-gel column was used for further clean up.The whole method has been evaluated on certified reference soil and farm soil.Accuracy and precision of this method was tested with satisfactory results.展开更多
Pentachlorphenol (PCP) was widely used as a biocide and insecticide for wood preservation. Chlorinated dioxins and furans (2,3,7,8-substituted PCDD and PCDF congeners) were inadvertent byproducts of PCP production. As...Pentachlorphenol (PCP) was widely used as a biocide and insecticide for wood preservation. Chlorinated dioxins and furans (2,3,7,8-substituted PCDD and PCDF congeners) were inadvertent byproducts of PCP production. As such, it is an important source of PCDD/F contamination in treated wood and in soil/ sediment near sites that produced or used PCP. It has been noted in the literature, that PCP congener profiles are similar to some combustion profiles, as well as sewage sludge and particulate deposition. In a very broad sense, this is true. OCDD and 1,2,3,4,6,7,8-HpCDD are typically the dominant constituents in these source categories. There is however, a distinct, consistent and repeatable feature in the lower chlorinated tetra, penta and hexa PCDD/F range of PCP related samples: an order of magnitude increase in concentration as a function of degree of chlorination. Because lower chlorinated furans concentrations make up less than 1% of the total PCDD/F in PCP, it is difficult to differentiate PCP from other OCDD dominated source profiles on bargraphs that use a linear-scale y axis. Using a log-scale y axis, however, PCP impacted profiles are obvious, and are not easily confused with congener profiles from other sources.展开更多
Since the 2010 s, the authorities of Guangdong province and local governments have enhanced law enforcement and environmental regulations to abolish open burning, acid washing, and other uncontrolled e-waste recycling...Since the 2010 s, the authorities of Guangdong province and local governments have enhanced law enforcement and environmental regulations to abolish open burning, acid washing, and other uncontrolled e-waste recycling activities. In this study, ambient air and indoor dust near different kinds of e-waste recycling processes were collected in Guiyu and Qingyuan to investigate the pollution status of particles and polychlorinated dibenzo-pdioxins and furans(PCDD/Fs) after stricter environmental regulations. PM_(2.5) and PCDD/Fs both showed significantly reduced levels in the two regions compared with the documented data. The congener distribution and principal component analysis results also confirmed the significant differences between the current PCDD/Fs pollution characterizations and the historical ones. The estimated total intake doses via air inhalation and dust ingestion of children in the recycling region of Guiyu ranged from 10 to 32 pg TEQ/(kg·day), which far exceeded the tolerable daily intake(TDI) limit(1–4 pg TEQ/(kg·day). Although the measurements showed a significant reduction of the release of PCDD/Fs, the pollution status was still considered severe in Guiyu town after stricter regulations were implemented.展开更多
Polychlorinated dibenzo-p-dioxins and furans(PCDD/Fs)generated from municipal solid waste(MSW)incineration are considered as the key pollutants,which could pose serious risks to the environment and ecology.This study ...Polychlorinated dibenzo-p-dioxins and furans(PCDD/Fs)generated from municipal solid waste(MSW)incineration are considered as the key pollutants,which could pose serious risks to the environment and ecology.This study comprehensively investigated the effect of selective catalytic reduction(SCR)system on PCDD/F removal,phase distributions,and migrationtransformation characteristics of 17 congeners in a full-scale MSW incinerator.The three flue gas samples and two fly ash samples were separately collected for PCDD/F analysis.The results showed that the SCR system reduced the I-TEQ concentration of PCDD/Fs from 0.135 to 0.010 ng I-TEQ Nm^(−3)with a remarkable toxicity removal efficiency of 92.6%,through oxidation decomposition over V_(2)O_(5)-WO_(3)/TiO_(2)catalysts and chlorination process of low-chlorinated congeners.In addition,the de novo synthesis observed along the flue between SCR system and stack regenerated unexpected PCDD/Fs,which might enhance the PCDD/F emission level.This study verified the three pathways of SCR system on PCDD/F removal and inspired operating suggestions for SCR system,i.e.,keeping SCR system operated in stable and consistent conditions,regularly replacing V_(2)O_(5)-WO_(3)/TiO_(2)catalysts,and timely cleaning the dusts and inlet materials of SCR system,which would be beneficial for achieving the ultra-low emission of PCDD/Fs in full-scale MSW incinerators.展开更多
A field study and theoretical calculations were performed to clarify the levels, profiles, and distributions of polybrominated dibenzo-p-dioxins and dibenzofurans(PBDD/Fs) in a cement kiln co-processing solid waste, w...A field study and theoretical calculations were performed to clarify the levels, profiles, and distributions of polybrominated dibenzo-p-dioxins and dibenzofurans(PBDD/Fs) in a cement kiln co-processing solid waste, with a focus on the PBDF formation mechanism.The raw materials contributed greatly to input of PBDD/Fs into the cement kiln. The PBDD/F concentrations in the raw materials were much higher than those in particle samples from different process stages in the cement kiln. The PBDD/F concentrations in the clinkers were1.40% of the concentrations in the raw materials, which indicated that the high destruction efficiencies for PBDD/Fs by cement kiln. PBDD/F distribution patterns in particle samples collected from different process stages indicated the cement kiln backend was a major site for PBDD/F formation. PBDFs with high levels of halogenation, such as heptabrominated furans(Hp BDF), were the dominant contributors to the total PBDD/F concentrations and accounted for 42%–73% of the total PBDD/F concentrations in the particle samples. Our results showed that co-processing of municipal solid waste in a cement kiln may influence the congener profile of PBDD/Fs, especially for the higher halogenated PBDD fraction. In addition, there were significant correlations between the decabromodiphenyl ether and heptabrominated furan concentrations, which is an indicator of transformation from polybrominated diphenyl ethers to PBDD/Fs. Theoretical calculations were performed and demonstrated that elimination of HBr and Br_2 from polybrominated diphenyl ethers were the dominant formation pathways for PBDD/Fs. These pathways differed from that for polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs).展开更多
文摘The research progress on the mechanisms of formation and degradation of polychlorinated dibenzo-p-dioxins ( PCDDs ) and dibenzofurans ( PCDFs ) is reviewed. The primary sources of PCDD/Fs are chemical, thermal, photochemical and enzymatic reactions. Most of the thermal sources result in emissions into air. The studies on the photodegradation and biodegradation offer promise for destruction of PCDD/Fs in environment.
文摘We analyzed polychlorinated dibenzofurans (PCDF) and dibenzo-p-dioxins (PCDD) in 27 tree bark samples from the industrialized area near Sauget, Illinois, USA. The trees were located within 4 km of the W. G. Krummrich (WGK) plant, the oldest and largest chemical plant in Sauget, with 24 of 27 samples collected from residential areas. The percent of total PCDF or PCDD profiles of ten 2,3,7,8- Cl substituted PCDF and seven PCDD congeners is homogeneous: 90% of the variance among the samples is explained by 3 eigenvalues in a principal components analysis. The homogeneity of the data suggests that samples were affected by similar types of sources which may have been influenced by electric power generation, chemical waste incineration, and large-scale thermal production of chlorinated chemicals. Quantitatively, the 2,3,7,8-Cl substituted congener analysis does not account for 90% of the concentration of tetra- and penta-Cl homologues and 80% of hexa-Cl and 50% of hepta-Cl homologues. The World Health Organization stated during establishment of toxic equivalence factors (TEF, 2005 version) that calculation of toxic equivalents (TEQs) is not suitable for abiotic matrices, such as tree bark, which are not involved in human exposures. Our results show that the non-2,3,7,8-Cl substituted congeners have high concentrations and should be included in analysis.
文摘Labeled polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)were extracted by three different methods,i.e.,soxhlet extraction,hot extraction and accelerated solvent extraction(ASE).The PCDD/Fs were detected by high resolution gas chromatography-high resolution mass spectrometry.Comparisons of the three methods were carried out by recovery of PCDD/Fs,solvent consumption and extraction time.The results showed that all of the method could extract labeled PCDD/Fs efficiently.ASE was a time saving procedure with lowest consumption of solvents compared with the other two methods.
文摘A rapid pretreatment method of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in soil and analysis by high resolution gas chromatograph-high resolution mass spectrometry was present.The extraction and alumina clean up of PCDD/Fs in soil was achieved by accelerated solvent extractor.Then the multi-layer silica-gel column was used for further clean up.The whole method has been evaluated on certified reference soil and farm soil.Accuracy and precision of this method was tested with satisfactory results.
文摘Pentachlorphenol (PCP) was widely used as a biocide and insecticide for wood preservation. Chlorinated dioxins and furans (2,3,7,8-substituted PCDD and PCDF congeners) were inadvertent byproducts of PCP production. As such, it is an important source of PCDD/F contamination in treated wood and in soil/ sediment near sites that produced or used PCP. It has been noted in the literature, that PCP congener profiles are similar to some combustion profiles, as well as sewage sludge and particulate deposition. In a very broad sense, this is true. OCDD and 1,2,3,4,6,7,8-HpCDD are typically the dominant constituents in these source categories. There is however, a distinct, consistent and repeatable feature in the lower chlorinated tetra, penta and hexa PCDD/F range of PCP related samples: an order of magnitude increase in concentration as a function of degree of chlorination. Because lower chlorinated furans concentrations make up less than 1% of the total PCDD/F in PCP, it is difficult to differentiate PCP from other OCDD dominated source profiles on bargraphs that use a linear-scale y axis. Using a log-scale y axis, however, PCP impacted profiles are obvious, and are not easily confused with congener profiles from other sources.
基金supported by the National Natural Science Foundation of China(No.91543202)the Ministry of Environmental Protection of the People's Republic of China(Nos.201409022,201409080 and 201509063)South China Institute of Environmental Science(No.PM-zx021-201510-015)
文摘Since the 2010 s, the authorities of Guangdong province and local governments have enhanced law enforcement and environmental regulations to abolish open burning, acid washing, and other uncontrolled e-waste recycling activities. In this study, ambient air and indoor dust near different kinds of e-waste recycling processes were collected in Guiyu and Qingyuan to investigate the pollution status of particles and polychlorinated dibenzo-pdioxins and furans(PCDD/Fs) after stricter environmental regulations. PM_(2.5) and PCDD/Fs both showed significantly reduced levels in the two regions compared with the documented data. The congener distribution and principal component analysis results also confirmed the significant differences between the current PCDD/Fs pollution characterizations and the historical ones. The estimated total intake doses via air inhalation and dust ingestion of children in the recycling region of Guiyu ranged from 10 to 32 pg TEQ/(kg·day), which far exceeded the tolerable daily intake(TDI) limit(1–4 pg TEQ/(kg·day). Although the measurements showed a significant reduction of the release of PCDD/Fs, the pollution status was still considered severe in Guiyu town after stricter regulations were implemented.
基金supported by the National Key R&D Program of China(Grant No. 2018YFC1902904)the National Natural Science Foundation of China (Grant No. 22008104)+4 种基金the Shenzhen Science and Technology Innovation Committee (Grant Nos. JCYJ20200109141642225,JCYJ20200109141227141, and JSGG20210713091810035)the Shenzhen Peacock Plan (Grant No. KQTD20160226195840229)provided by Basic and Applied Basic Research Foundation of Guangdong Province (Grant No. 2021A1515010148)Young S&T Talent Training Program of Guangdong Provincial Association for S&T(Grant No. SKXRC202230)Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2018
文摘Polychlorinated dibenzo-p-dioxins and furans(PCDD/Fs)generated from municipal solid waste(MSW)incineration are considered as the key pollutants,which could pose serious risks to the environment and ecology.This study comprehensively investigated the effect of selective catalytic reduction(SCR)system on PCDD/F removal,phase distributions,and migrationtransformation characteristics of 17 congeners in a full-scale MSW incinerator.The three flue gas samples and two fly ash samples were separately collected for PCDD/F analysis.The results showed that the SCR system reduced the I-TEQ concentration of PCDD/Fs from 0.135 to 0.010 ng I-TEQ Nm^(−3)with a remarkable toxicity removal efficiency of 92.6%,through oxidation decomposition over V_(2)O_(5)-WO_(3)/TiO_(2)catalysts and chlorination process of low-chlorinated congeners.In addition,the de novo synthesis observed along the flue between SCR system and stack regenerated unexpected PCDD/Fs,which might enhance the PCDD/F emission level.This study verified the three pathways of SCR system on PCDD/F removal and inspired operating suggestions for SCR system,i.e.,keeping SCR system operated in stable and consistent conditions,regularly replacing V_(2)O_(5)-WO_(3)/TiO_(2)catalysts,and timely cleaning the dusts and inlet materials of SCR system,which would be beneficial for achieving the ultra-low emission of PCDD/Fs in full-scale MSW incinerators.
基金supported by the National Natural Science Foundation of China(No.21777172)the Collaborative Project supported by Chinese Academy of Sciences and Hebei Academy of Sciences(No.181602)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2016038)
文摘A field study and theoretical calculations were performed to clarify the levels, profiles, and distributions of polybrominated dibenzo-p-dioxins and dibenzofurans(PBDD/Fs) in a cement kiln co-processing solid waste, with a focus on the PBDF formation mechanism.The raw materials contributed greatly to input of PBDD/Fs into the cement kiln. The PBDD/F concentrations in the raw materials were much higher than those in particle samples from different process stages in the cement kiln. The PBDD/F concentrations in the clinkers were1.40% of the concentrations in the raw materials, which indicated that the high destruction efficiencies for PBDD/Fs by cement kiln. PBDD/F distribution patterns in particle samples collected from different process stages indicated the cement kiln backend was a major site for PBDD/F formation. PBDFs with high levels of halogenation, such as heptabrominated furans(Hp BDF), were the dominant contributors to the total PBDD/F concentrations and accounted for 42%–73% of the total PBDD/F concentrations in the particle samples. Our results showed that co-processing of municipal solid waste in a cement kiln may influence the congener profile of PBDD/Fs, especially for the higher halogenated PBDD fraction. In addition, there were significant correlations between the decabromodiphenyl ether and heptabrominated furan concentrations, which is an indicator of transformation from polybrominated diphenyl ethers to PBDD/Fs. Theoretical calculations were performed and demonstrated that elimination of HBr and Br_2 from polybrominated diphenyl ethers were the dominant formation pathways for PBDD/Fs. These pathways differed from that for polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs).