Peat bogs are regarded as one of the faithful archives of atmospheric polycyclic aromatic hydrocarbons(PAHs) deposition, and a large number of studies on PAHs accumulation in peatlands have been reported in Europe and...Peat bogs are regarded as one of the faithful archives of atmospheric polycyclic aromatic hydrocarbons(PAHs) deposition, and a large number of studies on PAHs accumulation in peatlands have been reported in Europe and North America. Comparatively little information is available on peat chronological records of atmospheric PAHs flux in China. We investigated the concentrations and historical accumulation rates of PAHs(AR PAHs) through geochemical analysis of three 210Pb-dated ombrotrophic peat cores from Great Hinggan Mountain, northeast China. Eight USEPA priority PAHs were detected and they are naphthalene(Nap), acenaphthylene(Acl), acenaphthene(Ace), fluorence(Flu), phenanthrene(Phe), anthracene(Ant), fluoranthene(Fla) and pyrene(Pyr), respectively. The average total eight PAHs(tPAHs) concentrations are 135.98- 262.43 μg kg-1 and the average AR tPAHs over the last two centuries are 96.45- 135.98 μg m-2 yr-1. The Ace, Acl and Phe account for 30.93- 54.04%, 25.29- 35.81%, and 9.14- 19.84% of the tPAHs, respectively, and have significant positive correlations with the tPAH. As a result, they are regarded as the iconic compounds of PAHs pollution in this area. A ca.200-yr atmospheric PAHs contamination history was reconstructed from the temporal sequences of bothconcentration and AR tPAHs, suggesting the variation of local environmental pollution. The main sources of the PAHs are identified by two isomer ratios as petrogenic origin including oil extraction and refining process as well as their combustions for industrial development. In addition, the contribution of coal combustion for industrial activities and resident heating could not be ignored. But prior to 1860, the undeveloped industry and most of agricultural activities might mainly account for the low level of PAHs, although it could infer a long-range input of atmospheric PAHs from other industrial areas. Therefore, there is a global implication to study longterm PAHs pollution records and all the results will provide practical significance in formulating policies to achieve sustainable and healthy development.展开更多
Sixteen priority polycyclic aromatic hydrocarbons(PAHs) in surface water samples were analyzed by gas chromatograph-mass spectrometer(GC-MS) to study their distribution and characterizing sources.The water samples wer...Sixteen priority polycyclic aromatic hydrocarbons(PAHs) in surface water samples were analyzed by gas chromatograph-mass spectrometer(GC-MS) to study their distribution and characterizing sources.The water samples were collected from five sites(J1-J5) in the Jialing River of Chongqing downtown area from September 2009 to August 2010.The results demonstrate that the concentration of total PAHs in three samples upstream are relatively higher than those in other two sites downstream,with average concentration of total PAHs for each site ranging from 811.5 ng/L to 1585.8 ng/L.The 2,3 and 4-ring PAHs for sampling stations account for 13.0%,56.6% and 28.6%,respectively,in total PAHs.There are obvious tendencies of seasonal change for PAHs concentration in surface water.The PAHs concentration in April of wet season is 1 301.6 ng/L,which is 1.3 times the lowest amount of total PAHs in August of flood season.Ratios of specific PAH compounds were used to characterize the possible pollution sources.Experimental results indicate that the PAHs in surface water samples are primarily from pyrolytic PAHs because of factories along these sites,while the direct leakage of petroleum products may be significant for two sites,Jiahua Bridge(J4) and Huanghuayuan Bridge(J5),because of the wharf boat nearby.展开更多
Acylation reaction of anthracene with oxalyl chloride in the presence of [Emim]Cl-AlCl3 ionic liquid has been investigated. Pure 1,2-aceanthryenedione, which is used as intermediate of functional aromatic polymer mate...Acylation reaction of anthracene with oxalyl chloride in the presence of [Emim]Cl-AlCl3 ionic liquid has been investigated. Pure 1,2-aceanthryenedione, which is used as intermediate of functional aromatic polymer material, was obtained by recrystalling the reaction mixture with aether and was determined by GC/MS, 1↑HNMR and FTIR analysis. The influences of various parameters, such as the contents of AlCl3 in [Emim]Cl-AlCl3, the amount of acylation agent, amount of [Emim]Cl-AlCl3, reaction temperature and reaction time were investigated. The optimum conditions were as follows: the molar fraction of AlCl3 in ionic liquid [x(AlCl3)] being 0.67, molar ratio of ionic liquid to anthracene being 2:1, molar ratio of oxalyl chloride to anthracene being 2:1, reaction temperature being 40℃ and reaction time being 6h. Under above conditions, the yield and selectivity of 1,2-aceanthrylenedione can reach 91.5% and 98.3% respectively. Further more, [Emim]Cl-AlCl3 ionic liquid, compared with metal halides such as AlCl3, was found to catalyze the reaction as a novel environmental friendly catalyst and solvent and can be reused.展开更多
Acylation of anthracene and oxalyl chloride in the presence of anhydrous AlCl3 was investigated. Pure 1,2-aceanthrylenedione, which is used as new functional macromolecule, was prepared by extraction and recrystallati...Acylation of anthracene and oxalyl chloride in the presence of anhydrous AlCl3 was investigated. Pure 1,2-aceanthrylenedione, which is used as new functional macromolecule, was prepared by extraction and recrystallation. The structure of 1,2-aceanthrylenedione was identified by measure of melting point, GC/MS, FTIR and 1HNMR analyses. The influences of various parameters, such as solvent, dosage of catalyst, molar ratio of anthracene to oxalyl chloride, reaction temperature, and reaction time were studied. The anhydrous AlCl3 was found to catalyze the reaction with high yeild and good selectivity. When the reaction temperature is 303K, reaction time is 5h and molar ratio of anthracene to oxalyl chloride is 1:2, the yield and selectivity of 1,2-aceanthrylenedione is 83.8 % and 92.3% respectively.展开更多
Mixed contaminated brownfield sites have brought serious risks to human health and environmental safety. With the purpose of removing polycyclic aromatic hydrocarbons (PAHs) and heavy metals from a coking plant site...Mixed contaminated brownfield sites have brought serious risks to human health and environmental safety. With the purpose of removing polycyclic aromatic hydrocarbons (PAHs) and heavy metals from a coking plant site, an innovative technology for ex-situ washing was developed in the present work. The combination of 15.0 mLL-1 soybean oil and 7.5 g L-1 tea saponin proved an effective method to extract co-pollutants from soil. After two consecutive washing cycles, the efficiency rates of removal for 3-, 4-, 5(+6)-ring, and total PAHs, Cd, and Ni were approximately 98.2%, 96.4%, 92.3%, 96.3%, 94.1%, and 89.4%, respectively. Meanwhile, as evaluated by Tenax extraction method and metal stability indices, the residual PAHs and heavy metals after consecutive washing mainly existed in the form with extremely low bioaccessibility in the soil. Thus, in the soil after two washing cycles, there appeared limited environmental transfer risk of co-pollutants. Moreover, a subsequent precipitation method with alkaline solution and PAH- degrading strain Sphingobium sp. PHE9 inoculation effectively removed 84.6%-100% of Cd, 82.5%-91.7% of Ni, and 92.6%-98.4% of PAHs from the first and second washing solvents. The recovered solvents also exhibited a high recycling effectiveness. Therefore, the combined cleanup strategy proposed in this study proved environmentally friendly, which also played a major role in risk assessment and marlagement in mixed polluted sites.展开更多
基金funded by the National Natural Science Foundation of China(Grant No.4130121541271209)+1 种基金the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20131058)the National Basic Research Program of China(Grant No.2012CB956100)
文摘Peat bogs are regarded as one of the faithful archives of atmospheric polycyclic aromatic hydrocarbons(PAHs) deposition, and a large number of studies on PAHs accumulation in peatlands have been reported in Europe and North America. Comparatively little information is available on peat chronological records of atmospheric PAHs flux in China. We investigated the concentrations and historical accumulation rates of PAHs(AR PAHs) through geochemical analysis of three 210Pb-dated ombrotrophic peat cores from Great Hinggan Mountain, northeast China. Eight USEPA priority PAHs were detected and they are naphthalene(Nap), acenaphthylene(Acl), acenaphthene(Ace), fluorence(Flu), phenanthrene(Phe), anthracene(Ant), fluoranthene(Fla) and pyrene(Pyr), respectively. The average total eight PAHs(tPAHs) concentrations are 135.98- 262.43 μg kg-1 and the average AR tPAHs over the last two centuries are 96.45- 135.98 μg m-2 yr-1. The Ace, Acl and Phe account for 30.93- 54.04%, 25.29- 35.81%, and 9.14- 19.84% of the tPAHs, respectively, and have significant positive correlations with the tPAH. As a result, they are regarded as the iconic compounds of PAHs pollution in this area. A ca.200-yr atmospheric PAHs contamination history was reconstructed from the temporal sequences of bothconcentration and AR tPAHs, suggesting the variation of local environmental pollution. The main sources of the PAHs are identified by two isomer ratios as petrogenic origin including oil extraction and refining process as well as their combustions for industrial development. In addition, the contribution of coal combustion for industrial activities and resident heating could not be ignored. But prior to 1860, the undeveloped industry and most of agricultural activities might mainly account for the low level of PAHs, although it could infer a long-range input of atmospheric PAHs from other industrial areas. Therefore, there is a global implication to study longterm PAHs pollution records and all the results will provide practical significance in formulating policies to achieve sustainable and healthy development.
基金Project(41101457) supported by the National Natural Science Foundation of ChinaProject(2009-122) supported by the Fund of Chongqing Municipal Construction Commission, China
文摘Sixteen priority polycyclic aromatic hydrocarbons(PAHs) in surface water samples were analyzed by gas chromatograph-mass spectrometer(GC-MS) to study their distribution and characterizing sources.The water samples were collected from five sites(J1-J5) in the Jialing River of Chongqing downtown area from September 2009 to August 2010.The results demonstrate that the concentration of total PAHs in three samples upstream are relatively higher than those in other two sites downstream,with average concentration of total PAHs for each site ranging from 811.5 ng/L to 1585.8 ng/L.The 2,3 and 4-ring PAHs for sampling stations account for 13.0%,56.6% and 28.6%,respectively,in total PAHs.There are obvious tendencies of seasonal change for PAHs concentration in surface water.The PAHs concentration in April of wet season is 1 301.6 ng/L,which is 1.3 times the lowest amount of total PAHs in August of flood season.Ratios of specific PAH compounds were used to characterize the possible pollution sources.Experimental results indicate that the PAHs in surface water samples are primarily from pyrolytic PAHs because of factories along these sites,while the direct leakage of petroleum products may be significant for two sites,Jiahua Bridge(J4) and Huanghuayuan Bridge(J5),because of the wharf boat nearby.
基金National Natural Science Foundation of China (No.20207003)
文摘Acylation reaction of anthracene with oxalyl chloride in the presence of [Emim]Cl-AlCl3 ionic liquid has been investigated. Pure 1,2-aceanthryenedione, which is used as intermediate of functional aromatic polymer material, was obtained by recrystalling the reaction mixture with aether and was determined by GC/MS, 1↑HNMR and FTIR analysis. The influences of various parameters, such as the contents of AlCl3 in [Emim]Cl-AlCl3, the amount of acylation agent, amount of [Emim]Cl-AlCl3, reaction temperature and reaction time were investigated. The optimum conditions were as follows: the molar fraction of AlCl3 in ionic liquid [x(AlCl3)] being 0.67, molar ratio of ionic liquid to anthracene being 2:1, molar ratio of oxalyl chloride to anthracene being 2:1, reaction temperature being 40℃ and reaction time being 6h. Under above conditions, the yield and selectivity of 1,2-aceanthrylenedione can reach 91.5% and 98.3% respectively. Further more, [Emim]Cl-AlCl3 ionic liquid, compared with metal halides such as AlCl3, was found to catalyze the reaction as a novel environmental friendly catalyst and solvent and can be reused.
基金National Natural Science Foundation of China (No.20207003)
文摘Acylation of anthracene and oxalyl chloride in the presence of anhydrous AlCl3 was investigated. Pure 1,2-aceanthrylenedione, which is used as new functional macromolecule, was prepared by extraction and recrystallation. The structure of 1,2-aceanthrylenedione was identified by measure of melting point, GC/MS, FTIR and 1HNMR analyses. The influences of various parameters, such as solvent, dosage of catalyst, molar ratio of anthracene to oxalyl chloride, reaction temperature, and reaction time were studied. The anhydrous AlCl3 was found to catalyze the reaction with high yeild and good selectivity. When the reaction temperature is 303K, reaction time is 5h and molar ratio of anthracene to oxalyl chloride is 1:2, the yield and selectivity of 1,2-aceanthrylenedione is 83.8 % and 92.3% respectively.
基金financially supported by the Leading Project of the Institute of Soil Science, Chinese Academy of Sciences (ISSASIP1655)Jiangsu Municipal Natural Science Foundation, China (Nos. BK20141050 and BK20140723)the National Natural Science Foundation of China (Nos. 2014CB441105, 41401254, 41401347, and 41401345)
文摘Mixed contaminated brownfield sites have brought serious risks to human health and environmental safety. With the purpose of removing polycyclic aromatic hydrocarbons (PAHs) and heavy metals from a coking plant site, an innovative technology for ex-situ washing was developed in the present work. The combination of 15.0 mLL-1 soybean oil and 7.5 g L-1 tea saponin proved an effective method to extract co-pollutants from soil. After two consecutive washing cycles, the efficiency rates of removal for 3-, 4-, 5(+6)-ring, and total PAHs, Cd, and Ni were approximately 98.2%, 96.4%, 92.3%, 96.3%, 94.1%, and 89.4%, respectively. Meanwhile, as evaluated by Tenax extraction method and metal stability indices, the residual PAHs and heavy metals after consecutive washing mainly existed in the form with extremely low bioaccessibility in the soil. Thus, in the soil after two washing cycles, there appeared limited environmental transfer risk of co-pollutants. Moreover, a subsequent precipitation method with alkaline solution and PAH- degrading strain Sphingobium sp. PHE9 inoculation effectively removed 84.6%-100% of Cd, 82.5%-91.7% of Ni, and 92.6%-98.4% of PAHs from the first and second washing solvents. The recovered solvents also exhibited a high recycling effectiveness. Therefore, the combined cleanup strategy proposed in this study proved environmentally friendly, which also played a major role in risk assessment and marlagement in mixed polluted sites.