Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the...Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.展开更多
In the present work, the different sample collection, pretreatment and analytical methods for polycyclic aromatic hydrocarbons (PAHs) in airborne particulates is systematacially reviewed, and the applications of the...In the present work, the different sample collection, pretreatment and analytical methods for polycyclic aromatic hydrocarbons (PAHs) in airborne particulates is systematacially reviewed, and the applications of these pretreatment and analytical methods for PAHs are compared in detail. Some comments on the future expectation are also presented.展开更多
Sensitivity is crucially important for surface-enhanced Raman spectroscopy(SERS)application to detect trace-level polycyclic aromatic hydrocarbons(PAHs)in the seawater.In this study,a high sensitivity three-dimensiona...Sensitivity is crucially important for surface-enhanced Raman spectroscopy(SERS)application to detect trace-level polycyclic aromatic hydrocarbons(PAHs)in the seawater.In this study,a high sensitivity three-dimensional(3-D)SERS substrate composed with syringe filter,glycidyl methacrylate-ethylene dimethacrylate(GMA-EDMA)porous material and optimal parameters(57 nm,pH 13)gold nanoparticles(Au NPs)was developed for the detection of PAHs in water.The enhancement effect and repeatability of this 3-D substrate were also explored.The Raman intensity of pyrene using 3-D SERS substrate is about 8 times higher than that of substrate only using p H 13 gold colloid solution and about 12 times higher than that of substrate using natural Au NPs and GMA-EDMA porous material,which means both the pH 13 AuN Ps and the GMA-EDMA porous material are important factors for the sensitivity of this 3-D SERS substrate.Good repeatability of this optimal 3-D substrate was obtained.The relative standard deviation(RSD)is less than 8.66% on the same substrate and less than 3.69% on other different substrates.Four kinds of PAHs,i.e.,phenanthrene,pyrene,benzo(a)pyrene,benzo(k)fluoranthene and their mixture,were detected at the different concentrations.Their limits of detection(LODs)are 8.3×10^-10(phenanthrene),2.1×10^-10(pyrene),3.8×10^-10(benzo(a)pyrene)and 1.7×10^-10 mol L^-1(benzo(k)fluoranthene),respectively.In addition,these four PAHs were also detected by fluorescence spectroscopy to evaluate the sensitivity of SERS technology using this optimal 3-D SERS substrate.The results showed that the sensitivity of SERS based on the 3-D SERS substrate even using the portable Raman system was closed to that of fluorescence spectroscopy.Therefore,the SERS technology using this optimal 3-D substrate is expected to be an in-situ method for the detection of environmental PAHs.展开更多
Polycyclic aromatic hydrocarbons(PAHs)are one of the most important groups in oil,and re sponsible for major toxic and/or carcinogenic impact on humans and wildlife.It is important to understand the behavior of PAHs i...Polycyclic aromatic hydrocarbons(PAHs)are one of the most important groups in oil,and re sponsible for major toxic and/or carcinogenic impact on humans and wildlife.It is important to understand the behavior of PAHs in marine environment after an oil-spill incident.However,interaction between petroleum PAHs and microbial communities in a marine environment remains unclear.Therefore,a series of mesocosm experiments were conducted.in which water-accommodated fraction(WAF)of oil was generated to simulate an oil-spill scenario and to analyze the transport and behavior of marine oil spill containing PAHs with and without dispersants.Results indicate that the application of dispersant could increase the concentration of total PAHs in water column due mainly to significant increase in the concentration of highmolecular weight(HMW)PAHs at a lower removal rate.At the end of the 7-day experiment,significant amount of HMW PAHs were accumulated in sediment.In general,the application of dispersant did not increase the sediment uptake of PAHs but increased the PAHs concentration in water column.展开更多
This research aims to investigate the pollution characteristic of PAHs in Xiaodian sewage irrigation area. The result shows that the concentrations ofPAHs range from 47.94 to 46432.85ng/g while that of the total compo...This research aims to investigate the pollution characteristic of PAHs in Xiaodian sewage irrigation area. The result shows that the concentrations ofPAHs range from 47.94 to 46432.85ng/g while that of the total components of the 16 kinds of PAHs are 5969.81ng/g. PAHs with for rings and more than 4 rings are the main and important pollutants in topsoils of Xiaodian District. The main input of PAHs is combustion source, and the main pollution source in this area is fired coal. The topsoils in Xiaodian District are polluted by human activity in varying degrees. 23 of all 31 topsoil samples have been heavily polluted, especially those located nearby developed industrial townships and irrigation channels.展开更多
The present study was used freshwater Crab (Sesarma boulengeri Caiman) as bioindicator to measured the PAHs levels in AI-Hilla River, Iraq, during the period from March 2010 to February 2011. Crab samples were colle...The present study was used freshwater Crab (Sesarma boulengeri Caiman) as bioindicator to measured the PAHs levels in AI-Hilla River, Iraq, during the period from March 2010 to February 2011. Crab samples were collected from two sites on the AI-Hilla River. Sixteen of PAils compounds were identified seasonally in these samples. High mean value was (72.06 μg/g), recorded by Dibenzo (a, h) anthracene (DbA) in Site 1 and low mean value was (0.36 μg/g) recorded by Anthracene (Ant) in Site 2. The study showed a clear variation in PAHs concentration independent from the seasons and locations. Site 1 recorded high value of HMW (high molecular weight) and LMW (low molecular weight) more than Site 2. The present study revealed that all PAHs compounds were from Pyrogenic Origin. Seven carcinogenic PAHs (cPAHs) were recorded in crab tissues that were collected from the AI-Hilla River. The TEF (toxicity equivalency factor) was calculated to toxicity equivalent crab concentration. From the results, the fresh water Crab Sesarma boulengeri is a good bioindicator to water pollution by PAHs.展开更多
A new sampling method of ambient air analysis using carbonized fibrous resin as a sorbent for polycyclic aromatic hydrocarbons (PAHs) was reported. The physical and chemical properties of the carbonized fibrous resin...A new sampling method of ambient air analysis using carbonized fibrous resin as a sorbent for polycyclic aromatic hydrocarbons (PAHs) was reported. The physical and chemical properties of the carbonized fibrous resins were measured. The sample pretreatment with ultrasonic extraction and subsequent clean-up elution through a silica gel column was optimized. The suitable ultrasonic extraction conditions were selected as follows: resin weight was 1.5 g, ultrasonic extraction time 20 min, volume of extraction solvent 100 ml and extraction operation times 2~3. The concentrated extractable organic matter was submitted to next step of clean-up procedure of adsorption chromatography on silica gel column/n-hexane and a mixture of dichloromethene:n-hexane solution 2:3 (v/v). The PAHs fractions in the real samples from Changzhou, China were particularly analyzed using GC-MS data system and the data of mass spectra, retention times and scan numbers of the real samples were compared with that of the standards of 16 PAHs listed by the US EPA as 損riority pollutants?of the environment. The analysis of the real samples indicates that the carbonized fibrous resin is a good sorbent. The pretreatment of samples of ambient air with carbonized fibrous resin as a sorbent for PAHs is proved to be reliable and might be used for the procedure of the determination of PAHs in atmospheric environment.展开更多
[ Object] The aim was to discuss the pollution status of polycyclic aromatic hydrocarbons (PAHs) in mussels from the middle and lower main stream of Huaihe River, which will provide a scientific basis for dietary sa...[ Object] The aim was to discuss the pollution status of polycyclic aromatic hydrocarbons (PAHs) in mussels from the middle and lower main stream of Huaihe River, which will provide a scientific basis for dietary safety of mussels. [ Method] Suspended matter, sediment, and mussel samples were collected from Wuxiaojie and Fushanji in middle and lower reaches of Huaihe River. All samples were extracted with Soxhlet, separated through Silica GeI-Al2O3 column, and determined by GC-MS, and then 16 typical PAHs contents in the prior table listed by American EPA were obtained. [ Result] The results indicated that total PAHs concentrations in suspended matters and sediments of Wuxiaojie were significantly higher than those in Fushanji respectively. However, PAHs concentrations in mussels of the two samplings showed little difference; as for single PAH component, low-ring PAHs were more advantaged in suspended matters of two sampling sites, while high-ring PAHs were more advantaged in mussels. PAHs in sediments of Wuxiaojie assumed low-ring aspect, though PAHs in sediments of Fushanji assumed high-ring aspect. [ Conclusion] In spite of that sediments and mussels were not yet contaminated according to the ecological risk assessment of PAHs, its potential hazards couldn't be ignored any more.展开更多
The contents and distribution of 20 polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic hydrocarbons (HAHs) were investigated in 16 soil profiles of Beijing and Tianjin region. Transport of high mole...The contents and distribution of 20 polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic hydrocarbons (HAHs) were investigated in 16 soil profiles of Beijing and Tianjin region. Transport of high molecular weight PAHs (HMWPAHs) and the correlation between total organic carbon (TOC) and their concentrations were also discussed. The results indicated that highly contaminated sites were located at urban or wastewater irrigation areas and pollutants mainly accumulated in topsoil (〈 40 cm), with a sharp content decrease at the vertical boundary of 30-40 cm. Total PAHs/HAHs concentrations in soils from Tianjin were markedly greater than those from Beijing. Even the contents at bottoms of soil profiles in Tianjin were higher than those in topsoils of Beijing soil profile. HMWPAHs dominated the PAH profiles, exhibiting a uniform distribution of pyrogenic origin between topsoils and deep layers. Furthermore, the percentages of HMWPAHs remained relative constant with the depth of soil profiles, which were consistent with the distribution of particulate matter-associated PAHs in the local atmospheric environments. Therefore, HMWPAHs transport with particulates might be the predominant source found in soil profiles.展开更多
Pre-dried sewage sludge with high sulfur content was combusted in an electrically heated lab-scale fluidized-bed incinerator. The emission characteristics of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinate...Pre-dried sewage sludge with high sulfur content was combusted in an electrically heated lab-scale fluidized-bed incinerator. The emission characteristics of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polycyclic aromatic hydrocarbons (PAHs) were studied. Coal and calcium oxide (CaO) were added during the sewage sludge combustion tests to optimize combustion conditions and control SO2 emission. The results indicated that the flue gases emitted during mono-combustion of sewage sludge were characterized by relatively high concentrations of SO2, NOx and organic pollutants, due to the high sulfur, nitrogen, and volatile matter content of sewage sludge. The total 16 USEPA priority PAHs and 2,3,7,8-substituted PCDD/Fs produced from sewage sludge combustion were found to be 106.14 μg/m^3 and 8955.93 pg/m^3 in the flue gas, respectively. In the case of cocombustion with coal (msludge/mcoal =1:1), the 16 PAHs and 2,3,7,8-substituted PCDD/Fs concentrations were markedly lower than those found during mono-combustion of sewage sludge. During co-combustion, a suppressant effect of CaO on PCDD/Fs formation was observed.展开更多
A total of 11 PM2.5 samples were collected from October 2003 to October 2004 at 8 sampling sites in Beijing city. The PM2.5 concentrations are all above the PM2.5 pollution standard (65 μg m^-3) established by Envi...A total of 11 PM2.5 samples were collected from October 2003 to October 2004 at 8 sampling sites in Beijing city. The PM2.5 concentrations are all above the PM2.5 pollution standard (65 μg m^-3) established by Environmental Protection Agency, USA (USEPA) in 1997 except for the Ming Tombs site. PM2.5 concentrations in winter are much higher than in summer. The 16 Polycyclic aromatic hydrocarbons (PAHs) listed as priority pollutants by USEPA in PM2.5 were completely identified and quantified by high performance liquid chromatography (HPLC) with variable wavelength detector (VWD) and fluorescence detector (FLD) employed. The PM2.5 concentrations indicate that the pollution situation is still serious in Beijing. The sum of 16 PAHs concentrations ranged from 22.17 to 5366 ng m^-3. The concentrations of the heavier molecular weight PAHs have a different pollution trend from the lower PAHs. Seasonal variations were mainly attributed to the difference in coal combustion emission and meteorological conditions. The source apportionment analysis suggests that PAHs from PM2.5 in Beijing city mainly come from coal combustion and vehicle exhaust emission. New measures about restricting coal combustion and vehicle exhaust must be established as soon as possible to improve the air pollution situation in Beijing city.展开更多
We evaluated organic pollution in Bosten Lake, Xinjiang, China, by measuring the concentrations and distributions of organochlorine pesticides (OCPs) and polycyclic aromatic hydrocarbons (PAHs). Water and sediment...We evaluated organic pollution in Bosten Lake, Xinjiang, China, by measuring the concentrations and distributions of organochlorine pesticides (OCPs) and polycyclic aromatic hydrocarbons (PAHs). Water and sediment samples were collected from 19 sites 031-1319) in the lake for analysis. Our analytical results show that the concentrations of total OCPs in water ranges from 30.3 to 91.6 ng/L and the concentrations of PAHs ranges from undetectable (ND) to 368.7 ng/L. The concentrations of total OCPs in surface (i.e., lake bottom) sediment ranges from 6.9 to 16.7 ng/g and the concentrations of PAHs ranges from 25.2 to 491.0 ng/g. Hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) account for large proportions of the OCPs. Low α- to γ-HCH ratios in both water and sediment samples indicate possible contributions from both industrial products and lindane. DDTs in water are probably from historical input, whereas DDTs in sediments are from both historical and recent inputs. Moreover, DDT products in both water and sediments were from multiple sources in the northwestern part of the lake(B11, B12, B13, and B14). Fugacity ratios for DDT isomers (p,p'-DDE and p,p'-DDT) at these sites were generally higher than equilibrium values. These results suggest that the input from the Kaidu River and diffusion of DDTs from the sediment to the water are responsible for DDT pollution in the water. Lower-molecular-weight PAHs, which originate primarily from wood and coal combustion and petroleum sources, represent the major fraction of the PAHs in both water and sediment samples. Our findings indicate that OCPs and PAHs in Bosten Lake can be attributed primarily to human activities. A risk assessment of OCPs and PAHs in water and sediment from Bosten Lake, however, suggests that concentrations are not yet high enough to cause adverse biological effects on the aquatic ecosystem.展开更多
Atmospheric particulate and polycyclic aromatic hydrocarbons (PAHs) size distribution were measured at Jhu-Shan (a rural site) and Sin-Gang (a town site) in central Taiwan during the rice straw burning and non-b...Atmospheric particulate and polycyclic aromatic hydrocarbons (PAHs) size distribution were measured at Jhu-Shan (a rural site) and Sin-Gang (a town site) in central Taiwan during the rice straw burning and non-burning periods. The concentrations of total PAHs accounting for a roughly 58% (34%) increment in the concentrations of total PAHs due to rice-straw burning. Combustion-related PAHs during burning periods were 1.54-2.57 times higher than those during non-burning periods. The mass median diameter (MMD) of 0.88-1.21 μm in the particulate phase suggested that rice-straw burning generated the increase in coarse particle number. Chemical mass balance (CMB) receptor model analyses showed that the primary pollution sources at the two sites were similar. However, ricestraw burning emission was specifically identified as a significant source of PAH during burning periods at the two sites. Open burning of rice straws was estimated to contribute approximately 6.3%-24.6% to total atmospheric PAHs at the two sites.展开更多
This study examined the concentrations of polycyclic aromatic hydrocarbons (PAHs) in surface sediments collected in July 2004 from eight stations in the Zhelin Bay, one of the most important bays for large-scale mar...This study examined the concentrations of polycyclic aromatic hydrocarbons (PAHs) in surface sediments collected in July 2004 from eight stations in the Zhelin Bay, one of the most important bays for large-scale mariculture in Guangdong Province. Thirteen individual parent PAH compounds were identified using high performance liquid chromatography with UV detection. The overall average concentration of total PAHs was 477.0 ng/g, ranging from 146.1 to 928.8 ng/g. Low molecular mass PAHs with two to three rings (e.g., acenaphthene) were dominant in each sample. The PAH concentration varied among sampling stations, with the highest concentration observed at bay outlets and the lowest found at stations outside the bay. Ratios of low to high molecular mass PAHs and fluoranthene to pyrene were used to determine the origin of PAHs, and results indicated mainly petroleum-derived contamination. Compared with other bays and harbors around the world, the total concentrations of PAHs in surface sediments at the Zhelin Bay are moderate, but this does not exclude the possibility of potential impact on human consumers because some strong carcinogenic PAHs with high molecular mass were found at the station with a nearby caged-fish and oyster farm. Long-term monitoring of PAH contamination in the Zhelin Bay is recommended to reduce the potential toxicological effects on aquatic: organisms and humans.展开更多
Polycyclic aromatic hydrocarbons (PAHs) are potentially carcinogenic and mutagenic compounds that have raised considerable environmental concern. The highest concentrations of PAHs in the coastal sediment samples in C...Polycyclic aromatic hydrocarbons (PAHs) are potentially carcinogenic and mutagenic compounds that have raised considerable environmental concern. The highest concentrations of PAHs in the coastal sediment samples in China was 5.8-11.0μg/g (dry weight) in the core from the Huangpu River, Shanghai. The second highest concentration of PAHs was 4.42μg/g (dry weight) in surface sediment of Victoria Harbour in Hong Kong, and 5.73μg/g (dry weight) in sediment of Jiaozhou Bay, Qingdao City. The low concentrations of PAHs were always in the sediments far away from industrial zones and cities, and ranged from 0.10 to 0.30μg/g (dry weight). Several environmental parameters are considered for the identification of sources of PAHs in marine environment. High proportion of naphthalene, low molecular weight PAHs and alkylated PAHs, plus high ratio of phenanthrene to anthracene (>15) and low ratio of fluoranthene to pyrene (<1) suggested a petrogenic source. According to these parameters, the Changjiang (Yangtze) River estuary of Shanghai, Jiaozhou Bay of Qingdao City, Zhujiang (Pearl) River mouth, Jiulong River mouth and most of Hong Kong coastal waters were heavily contaminated by PAHs from petrogenic sources. However, PAHs in rural coastal areas were dominated by pyrolytic origin PAHs. This review clearly showed that oil pollution and incomplete combustion of oil, coal and biomass are the main reason for PAHs anormalies in the study areas.展开更多
Tunnel wash waters characterize all waters that run off after washing procedures of tunnels are performed.These waters represent a wide spectrum of organic and inorganic pollutants,such as polycyclic aromatic hydrocar...Tunnel wash waters characterize all waters that run off after washing procedures of tunnels are performed.These waters represent a wide spectrum of organic and inorganic pollutants,such as polycyclic aromatic hydrocarbons(PAHs)and toxic metals.Removal of such contaminants from water runoff was investigated using laboratory tests after washing procedure was performed on two road tunnels in eastern Norway(Hanekleiv and Bragernes).Due to diverse character of both,treatment media and treated wash waters, the wh...展开更多
[Method] This study aimed to determine trace amount of polycyclic aromatic hydrocarbons(PAHs) in urban sewage by using solid-phase extraction(SPE) coupled with high performance liquid chromatograph(HPLC).[Method] From...[Method] This study aimed to determine trace amount of polycyclic aromatic hydrocarbons(PAHs) in urban sewage by using solid-phase extraction(SPE) coupled with high performance liquid chromatograph(HPLC).[Method] From the aspects of solid-phase extraction column,elution solvent,elution volume,elution speed and so forth,the test conditions of SPE-HPLC method were optimized,and trace amount of PAHs in urban sewage was determined.[Result] The optimized solid-phase extraction conditions were SUPELCLEAN LC-18 solid-phase extraction column,methylene dichloride as elution solvent,15 ml elution volume,2 ml/min elution speed,5 ml/min loading speed,1 000 ml water with 200 ml methanol loading volume.Under the optimized extraction conditions,the recovery was high,namely 76.3%-105.2%;relative standard deviation was 3.8%-6.0%,showing good precision;detection limit was low,only 0.000 8-0.048 0 μg/L.[Conclusion] This method is user-friendly,with high sensitivity and good precision,and suitable for continuous determination of a large volume of water samples.展开更多
基金financial support from the National Natural Science Foundation of China(21991092,21991090,22022202,21972142,21902153,21974138)the Chinese Academy of Sciences(QYZDY-SSW-SC024)the Dalian Institute of Chemical Physics(DICP I201926,DICP I201947)。
文摘Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.
基金Project supported by the National Natural Science Foundation of China (No. 20437020 20575073) NSFC-JSPS Joint Research Project (No. 20511140134) the Major Research Program of Chinese Academy of Sciences (KZCX3-SW-432)
文摘In the present work, the different sample collection, pretreatment and analytical methods for polycyclic aromatic hydrocarbons (PAHs) in airborne particulates is systematacially reviewed, and the applications of these pretreatment and analytical methods for PAHs are compared in detail. Some comments on the future expectation are also presented.
基金supported by the National Natural Science Foundation of China (No. 41476081)the Major Research and Development Project in Shandong Province (Nos. 2016GSF115020, 2019GHY112027)the Shandong Provincial Natural Science Foundation (No. ZR2015DM007)
文摘Sensitivity is crucially important for surface-enhanced Raman spectroscopy(SERS)application to detect trace-level polycyclic aromatic hydrocarbons(PAHs)in the seawater.In this study,a high sensitivity three-dimensional(3-D)SERS substrate composed with syringe filter,glycidyl methacrylate-ethylene dimethacrylate(GMA-EDMA)porous material and optimal parameters(57 nm,pH 13)gold nanoparticles(Au NPs)was developed for the detection of PAHs in water.The enhancement effect and repeatability of this 3-D substrate were also explored.The Raman intensity of pyrene using 3-D SERS substrate is about 8 times higher than that of substrate only using p H 13 gold colloid solution and about 12 times higher than that of substrate using natural Au NPs and GMA-EDMA porous material,which means both the pH 13 AuN Ps and the GMA-EDMA porous material are important factors for the sensitivity of this 3-D SERS substrate.Good repeatability of this optimal 3-D substrate was obtained.The relative standard deviation(RSD)is less than 8.66% on the same substrate and less than 3.69% on other different substrates.Four kinds of PAHs,i.e.,phenanthrene,pyrene,benzo(a)pyrene,benzo(k)fluoranthene and their mixture,were detected at the different concentrations.Their limits of detection(LODs)are 8.3×10^-10(phenanthrene),2.1×10^-10(pyrene),3.8×10^-10(benzo(a)pyrene)and 1.7×10^-10 mol L^-1(benzo(k)fluoranthene),respectively.In addition,these four PAHs were also detected by fluorescence spectroscopy to evaluate the sensitivity of SERS technology using this optimal 3-D SERS substrate.The results showed that the sensitivity of SERS based on the 3-D SERS substrate even using the portable Raman system was closed to that of fluorescence spectroscopy.Therefore,the SERS technology using this optimal 3-D substrate is expected to be an in-situ method for the detection of environmental PAHs.
文摘Polycyclic aromatic hydrocarbons(PAHs)are one of the most important groups in oil,and re sponsible for major toxic and/or carcinogenic impact on humans and wildlife.It is important to understand the behavior of PAHs in marine environment after an oil-spill incident.However,interaction between petroleum PAHs and microbial communities in a marine environment remains unclear.Therefore,a series of mesocosm experiments were conducted.in which water-accommodated fraction(WAF)of oil was generated to simulate an oil-spill scenario and to analyze the transport and behavior of marine oil spill containing PAHs with and without dispersants.Results indicate that the application of dispersant could increase the concentration of total PAHs in water column due mainly to significant increase in the concentration of highmolecular weight(HMW)PAHs at a lower removal rate.At the end of the 7-day experiment,significant amount of HMW PAHs were accumulated in sediment.In general,the application of dispersant did not increase the sediment uptake of PAHs but increased the PAHs concentration in water column.
文摘This research aims to investigate the pollution characteristic of PAHs in Xiaodian sewage irrigation area. The result shows that the concentrations ofPAHs range from 47.94 to 46432.85ng/g while that of the total components of the 16 kinds of PAHs are 5969.81ng/g. PAHs with for rings and more than 4 rings are the main and important pollutants in topsoils of Xiaodian District. The main input of PAHs is combustion source, and the main pollution source in this area is fired coal. The topsoils in Xiaodian District are polluted by human activity in varying degrees. 23 of all 31 topsoil samples have been heavily polluted, especially those located nearby developed industrial townships and irrigation channels.
文摘The present study was used freshwater Crab (Sesarma boulengeri Caiman) as bioindicator to measured the PAHs levels in AI-Hilla River, Iraq, during the period from March 2010 to February 2011. Crab samples were collected from two sites on the AI-Hilla River. Sixteen of PAils compounds were identified seasonally in these samples. High mean value was (72.06 μg/g), recorded by Dibenzo (a, h) anthracene (DbA) in Site 1 and low mean value was (0.36 μg/g) recorded by Anthracene (Ant) in Site 2. The study showed a clear variation in PAHs concentration independent from the seasons and locations. Site 1 recorded high value of HMW (high molecular weight) and LMW (low molecular weight) more than Site 2. The present study revealed that all PAHs compounds were from Pyrogenic Origin. Seven carcinogenic PAHs (cPAHs) were recorded in crab tissues that were collected from the AI-Hilla River. The TEF (toxicity equivalency factor) was calculated to toxicity equivalent crab concentration. From the results, the fresh water Crab Sesarma boulengeri is a good bioindicator to water pollution by PAHs.
基金The Natural Science Foundation of Jangsu Province. No. BK93124313
文摘A new sampling method of ambient air analysis using carbonized fibrous resin as a sorbent for polycyclic aromatic hydrocarbons (PAHs) was reported. The physical and chemical properties of the carbonized fibrous resins were measured. The sample pretreatment with ultrasonic extraction and subsequent clean-up elution through a silica gel column was optimized. The suitable ultrasonic extraction conditions were selected as follows: resin weight was 1.5 g, ultrasonic extraction time 20 min, volume of extraction solvent 100 ml and extraction operation times 2~3. The concentrated extractable organic matter was submitted to next step of clean-up procedure of adsorption chromatography on silica gel column/n-hexane and a mixture of dichloromethene:n-hexane solution 2:3 (v/v). The PAHs fractions in the real samples from Changzhou, China were particularly analyzed using GC-MS data system and the data of mass spectra, retention times and scan numbers of the real samples were compared with that of the standards of 16 PAHs listed by the US EPA as 損riority pollutants?of the environment. The analysis of the real samples indicates that the carbonized fibrous resin is a good sorbent. The pretreatment of samples of ambient air with carbonized fibrous resin as a sorbent for PAHs is proved to be reliable and might be used for the procedure of the determination of PAHs in atmospheric environment.
基金Supported by the National Natural Science Foundation of China(No.40073030)~~
文摘[ Object] The aim was to discuss the pollution status of polycyclic aromatic hydrocarbons (PAHs) in mussels from the middle and lower main stream of Huaihe River, which will provide a scientific basis for dietary safety of mussels. [ Method] Suspended matter, sediment, and mussel samples were collected from Wuxiaojie and Fushanji in middle and lower reaches of Huaihe River. All samples were extracted with Soxhlet, separated through Silica GeI-Al2O3 column, and determined by GC-MS, and then 16 typical PAHs contents in the prior table listed by American EPA were obtained. [ Result] The results indicated that total PAHs concentrations in suspended matters and sediments of Wuxiaojie were significantly higher than those in Fushanji respectively. However, PAHs concentrations in mussels of the two samplings showed little difference; as for single PAH component, low-ring PAHs were more advantaged in suspended matters of two sampling sites, while high-ring PAHs were more advantaged in mussels. PAHs in sediments of Wuxiaojie assumed low-ring aspect, though PAHs in sediments of Fushanji assumed high-ring aspect. [ Conclusion] In spite of that sediments and mussels were not yet contaminated according to the ecological risk assessment of PAHs, its potential hazards couldn't be ignored any more.
基金supported by the National NaturalScience Foundation of China (No. 40473045)
文摘The contents and distribution of 20 polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic hydrocarbons (HAHs) were investigated in 16 soil profiles of Beijing and Tianjin region. Transport of high molecular weight PAHs (HMWPAHs) and the correlation between total organic carbon (TOC) and their concentrations were also discussed. The results indicated that highly contaminated sites were located at urban or wastewater irrigation areas and pollutants mainly accumulated in topsoil (〈 40 cm), with a sharp content decrease at the vertical boundary of 30-40 cm. Total PAHs/HAHs concentrations in soils from Tianjin were markedly greater than those from Beijing. Even the contents at bottoms of soil profiles in Tianjin were higher than those in topsoils of Beijing soil profile. HMWPAHs dominated the PAH profiles, exhibiting a uniform distribution of pyrogenic origin between topsoils and deep layers. Furthermore, the percentages of HMWPAHs remained relative constant with the depth of soil profiles, which were consistent with the distribution of particulate matter-associated PAHs in the local atmospheric environments. Therefore, HMWPAHs transport with particulates might be the predominant source found in soil profiles.
基金supported by the Important Project on Science and Technology of Zhejiang Province of China(No. 2007C03003)the National Natural Science Foundation of China (No. 50576082)
文摘Pre-dried sewage sludge with high sulfur content was combusted in an electrically heated lab-scale fluidized-bed incinerator. The emission characteristics of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polycyclic aromatic hydrocarbons (PAHs) were studied. Coal and calcium oxide (CaO) were added during the sewage sludge combustion tests to optimize combustion conditions and control SO2 emission. The results indicated that the flue gases emitted during mono-combustion of sewage sludge were characterized by relatively high concentrations of SO2, NOx and organic pollutants, due to the high sulfur, nitrogen, and volatile matter content of sewage sludge. The total 16 USEPA priority PAHs and 2,3,7,8-substituted PCDD/Fs produced from sewage sludge combustion were found to be 106.14 μg/m^3 and 8955.93 pg/m^3 in the flue gas, respectively. In the case of cocombustion with coal (msludge/mcoal =1:1), the 16 PAHs and 2,3,7,8-substituted PCDD/Fs concentrations were markedly lower than those found during mono-combustion of sewage sludge. During co-combustion, a suppressant effect of CaO on PCDD/Fs formation was observed.
基金Financial support from the National Natural Science Foundation of China (Grant No. 40475049) the Natural Sciences Foundation of Beijing city (Grant No. 8032012) are acknowledged.
文摘A total of 11 PM2.5 samples were collected from October 2003 to October 2004 at 8 sampling sites in Beijing city. The PM2.5 concentrations are all above the PM2.5 pollution standard (65 μg m^-3) established by Environmental Protection Agency, USA (USEPA) in 1997 except for the Ming Tombs site. PM2.5 concentrations in winter are much higher than in summer. The 16 Polycyclic aromatic hydrocarbons (PAHs) listed as priority pollutants by USEPA in PM2.5 were completely identified and quantified by high performance liquid chromatography (HPLC) with variable wavelength detector (VWD) and fluorescence detector (FLD) employed. The PM2.5 concentrations indicate that the pollution situation is still serious in Beijing. The sum of 16 PAHs concentrations ranged from 22.17 to 5366 ng m^-3. The concentrations of the heavier molecular weight PAHs have a different pollution trend from the lower PAHs. Seasonal variations were mainly attributed to the difference in coal combustion emission and meteorological conditions. The source apportionment analysis suggests that PAHs from PM2.5 in Beijing city mainly come from coal combustion and vehicle exhaust emission. New measures about restricting coal combustion and vehicle exhaust must be established as soon as possible to improve the air pollution situation in Beijing city.
基金funded by the National Natural Science Foundation of China(4147117341671200+1 种基金U1603242)the Specific Scientific Research Fund from the Ministry of Environmental Protection of the People’s Republic of China(201309041)
文摘We evaluated organic pollution in Bosten Lake, Xinjiang, China, by measuring the concentrations and distributions of organochlorine pesticides (OCPs) and polycyclic aromatic hydrocarbons (PAHs). Water and sediment samples were collected from 19 sites 031-1319) in the lake for analysis. Our analytical results show that the concentrations of total OCPs in water ranges from 30.3 to 91.6 ng/L and the concentrations of PAHs ranges from undetectable (ND) to 368.7 ng/L. The concentrations of total OCPs in surface (i.e., lake bottom) sediment ranges from 6.9 to 16.7 ng/g and the concentrations of PAHs ranges from 25.2 to 491.0 ng/g. Hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) account for large proportions of the OCPs. Low α- to γ-HCH ratios in both water and sediment samples indicate possible contributions from both industrial products and lindane. DDTs in water are probably from historical input, whereas DDTs in sediments are from both historical and recent inputs. Moreover, DDT products in both water and sediments were from multiple sources in the northwestern part of the lake(B11, B12, B13, and B14). Fugacity ratios for DDT isomers (p,p'-DDE and p,p'-DDT) at these sites were generally higher than equilibrium values. These results suggest that the input from the Kaidu River and diffusion of DDTs from the sediment to the water are responsible for DDT pollution in the water. Lower-molecular-weight PAHs, which originate primarily from wood and coal combustion and petroleum sources, represent the major fraction of the PAHs in both water and sediment samples. Our findings indicate that OCPs and PAHs in Bosten Lake can be attributed primarily to human activities. A risk assessment of OCPs and PAHs in water and sediment from Bosten Lake, however, suggests that concentrations are not yet high enough to cause adverse biological effects on the aquatic ecosystem.
基金The Central Taiwan University of Science and Technology supported this work under the grant 94-INS-024
文摘Atmospheric particulate and polycyclic aromatic hydrocarbons (PAHs) size distribution were measured at Jhu-Shan (a rural site) and Sin-Gang (a town site) in central Taiwan during the rice straw burning and non-burning periods. The concentrations of total PAHs accounting for a roughly 58% (34%) increment in the concentrations of total PAHs due to rice-straw burning. Combustion-related PAHs during burning periods were 1.54-2.57 times higher than those during non-burning periods. The mass median diameter (MMD) of 0.88-1.21 μm in the particulate phase suggested that rice-straw burning generated the increase in coarse particle number. Chemical mass balance (CMB) receptor model analyses showed that the primary pollution sources at the two sites were similar. However, ricestraw burning emission was specifically identified as a significant source of PAH during burning periods at the two sites. Open burning of rice straws was estimated to contribute approximately 6.3%-24.6% to total atmospheric PAHs at the two sites.
基金This work was funded by the National Natural Science Foundation of China under contract No.40176029.
文摘This study examined the concentrations of polycyclic aromatic hydrocarbons (PAHs) in surface sediments collected in July 2004 from eight stations in the Zhelin Bay, one of the most important bays for large-scale mariculture in Guangdong Province. Thirteen individual parent PAH compounds were identified using high performance liquid chromatography with UV detection. The overall average concentration of total PAHs was 477.0 ng/g, ranging from 146.1 to 928.8 ng/g. Low molecular mass PAHs with two to three rings (e.g., acenaphthene) were dominant in each sample. The PAH concentration varied among sampling stations, with the highest concentration observed at bay outlets and the lowest found at stations outside the bay. Ratios of low to high molecular mass PAHs and fluoranthene to pyrene were used to determine the origin of PAHs, and results indicated mainly petroleum-derived contamination. Compared with other bays and harbors around the world, the total concentrations of PAHs in surface sediments at the Zhelin Bay are moderate, but this does not exclude the possibility of potential impact on human consumers because some strong carcinogenic PAHs with high molecular mass were found at the station with a nearby caged-fish and oyster farm. Long-term monitoring of PAH contamination in the Zhelin Bay is recommended to reduce the potential toxicological effects on aquatic: organisms and humans.
文摘Polycyclic aromatic hydrocarbons (PAHs) are potentially carcinogenic and mutagenic compounds that have raised considerable environmental concern. The highest concentrations of PAHs in the coastal sediment samples in China was 5.8-11.0μg/g (dry weight) in the core from the Huangpu River, Shanghai. The second highest concentration of PAHs was 4.42μg/g (dry weight) in surface sediment of Victoria Harbour in Hong Kong, and 5.73μg/g (dry weight) in sediment of Jiaozhou Bay, Qingdao City. The low concentrations of PAHs were always in the sediments far away from industrial zones and cities, and ranged from 0.10 to 0.30μg/g (dry weight). Several environmental parameters are considered for the identification of sources of PAHs in marine environment. High proportion of naphthalene, low molecular weight PAHs and alkylated PAHs, plus high ratio of phenanthrene to anthracene (>15) and low ratio of fluoranthene to pyrene (<1) suggested a petrogenic source. According to these parameters, the Changjiang (Yangtze) River estuary of Shanghai, Jiaozhou Bay of Qingdao City, Zhujiang (Pearl) River mouth, Jiulong River mouth and most of Hong Kong coastal waters were heavily contaminated by PAHs from petrogenic sources. However, PAHs in rural coastal areas were dominated by pyrolytic origin PAHs. This review clearly showed that oil pollution and incomplete combustion of oil, coal and biomass are the main reason for PAHs anormalies in the study areas.
文摘Tunnel wash waters characterize all waters that run off after washing procedures of tunnels are performed.These waters represent a wide spectrum of organic and inorganic pollutants,such as polycyclic aromatic hydrocarbons(PAHs)and toxic metals.Removal of such contaminants from water runoff was investigated using laboratory tests after washing procedure was performed on two road tunnels in eastern Norway(Hanekleiv and Bragernes).Due to diverse character of both,treatment media and treated wash waters, the wh...
基金Supported by National Science and Technology Key Project of Water Pollution Control and Management (2012ZX07209-003)
文摘[Method] This study aimed to determine trace amount of polycyclic aromatic hydrocarbons(PAHs) in urban sewage by using solid-phase extraction(SPE) coupled with high performance liquid chromatograph(HPLC).[Method] From the aspects of solid-phase extraction column,elution solvent,elution volume,elution speed and so forth,the test conditions of SPE-HPLC method were optimized,and trace amount of PAHs in urban sewage was determined.[Result] The optimized solid-phase extraction conditions were SUPELCLEAN LC-18 solid-phase extraction column,methylene dichloride as elution solvent,15 ml elution volume,2 ml/min elution speed,5 ml/min loading speed,1 000 ml water with 200 ml methanol loading volume.Under the optimized extraction conditions,the recovery was high,namely 76.3%-105.2%;relative standard deviation was 3.8%-6.0%,showing good precision;detection limit was low,only 0.000 8-0.048 0 μg/L.[Conclusion] This method is user-friendly,with high sensitivity and good precision,and suitable for continuous determination of a large volume of water samples.