Chlorine source is indispensable for polychlorinated dibenzo-p-dioxin and furan (PCDD/F) formation during municipal solid waste (MSW) incineration. Inorganic chlorine compounds were employed in this study to inves...Chlorine source is indispensable for polychlorinated dibenzo-p-dioxin and furan (PCDD/F) formation during municipal solid waste (MSW) incineration. Inorganic chlorine compounds were employed in this study to investigate their effects on PCDD/F formation through heterogeneous synthesis on fly ash surfaces. A fly ash sample obtained from a fluidized bed incinerator was sieved to different size fractions which served as the PCDD/F formation sources. The capability of different metal chlorides which facilitate the formation of PCDDs/Fs was found to follow the trends: Na 〈 Mg 〈 K 〈 AI 〈 Ca, when two particle fractions of 〉177 μm and 104-125 μm were used in the experiments. However, the capability of NaCI, MgCl2 and KCI did not seem much different from each other, whereas CaCl2 and AlCl3 were much more active in PCDD/F formation. NaCl and MgCl2 were relatively effective to produce more PCDDs, while KC1, AICl3 and CaCl2 generated more PCDFs during heterogeneous reactions occurring on fly ash. 2,3,7,8-TCDF was the most significant contributor to the toxicity of the PCDDs/Fs formed from inorganic chlorine sources. Decreasing the sizes of fly ash particles led to more active formation of PCDDs/Fs when NaCl was used as inorganic chlorine in the experiment. The highest PCDDs/Fs produced from particles with size 〈37 μm, while the lowest PCDDs/Fs produced from particles with size 〉177μm. The toxicity generally increased with decreasing size of the fly ash particles. The formation of PCDDs was mainly facilitated by the two size fractions, 104-125 μm and 〈37μm, while the formation of PCDFs was favored by the two other size fractions, 〉177 μm and 53-104 μm.展开更多
In January 2013, a long-lasting severe haze episode occurred in Northern and Central China; at its maximum, it covered a land area of approximately 1.4 million km2. In Wuhan, the largest city in Central China, this ev...In January 2013, a long-lasting severe haze episode occurred in Northern and Central China; at its maximum, it covered a land area of approximately 1.4 million km2. In Wuhan, the largest city in Central China, this event was the most severe haze episode in the 21st century. Aerosol samples of submicron particles (PMI.o) were collected during the long-lasting haze episode at an urban site and a suburban site in Wuhan to investigate the ion characteristics of PMi.0 in this area. The mass concentrations of PM1.0 and its water-soluble inorganic ions (WSIIs) were almost at the same levels at two sites, which indicates that PM1.0 pollution occurs on a regional scale in Wuhao. WSIIs (Na^+, NH4^+, K^+, Mg^2+, Ca^2+, Cl^-, NO3 and SO2-) were the dominant chemical species and constituted up to 48.4% and 47.4% of PM1.0 at WD and TH, respectively. The concentrations of PM1.0 and WSIIs on haze days were approximately two times higher than on normal days. The ion balance calculations indicate that the particles were more acidic on haze days than on normal days. The results of the back trajectory analysis imply that the high concentrations of PM1.0 and its water-soluble inorganic ions may be caused by stagnant weather conditions in Wuhan.展开更多
In this study, we performed a highly time-resolved chemical characterization of nonrefractory submicron particles(NR-PM_1) in Beijing by using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer(HR...In this study, we performed a highly time-resolved chemical characterization of nonrefractory submicron particles(NR-PM_1) in Beijing by using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer(HR-ToF-AMS). The results showed the average NR-PM_1 mass concentration to be 56.4 ± 58.0 μg/m^3, with a peak at 307.4 μg/m^3. Due to the high frequency of biomass burning in autumn, submicron particles significantly increased in organic content, which accounted for 51% of NR-PM_1 on average. Secondary inorganic aerosols(sulfate + nitrate + ammonium) accounted for 46% of NR-PM_1, of which sulfate,nitrate, and ammonium contributed 15%, 20%, and 11%, respectively. To determine the intrinsic relationships between the organic and inorganic species, we used the positive matrix factorization(PMF) model to merge the high-resolution mass spectra of the organic species and NO+and NO_2~+ions. The PMF analysis separated the mixed organic and nitrate(NO+and NO_2~+) spectra into four organic factors, including hydrocarbon-like organic aerosol(HOA), oxygenated organic aerosol(OOA), cooking organic aerosol(COA), and biomass burning organic aerosol(BBOA), as well as one nitrate inorganic aerosol(NIA) factor. COA(33%) and OOA(30%) contributed the most to the total organic aerosol(OA) mass, followed by BBOA(20%) and HOA(17%). We successfully quantified the mass concentrations of the organic and inorganic nitrates by the NO+and NO2+ions signal in the organic and NIA factors. The organic nitrate mass varied from 0.01-6.8 μg/m^3, with an average of 1.0 ±1.1 μg/m^3, and organic nitrate components accounted for 10% of the total nitrate mass in this observation.展开更多
基金Project supported by the National Natural Science Foundation of China(No.59878047)the National Key Basic Research Special Funds Projectof China(No.1999022211)+1 种基金the Key Project of National Natural Science Foundation(No.59836210)Zhejiang Province Natural Science Foundation(No.X206955).
文摘Chlorine source is indispensable for polychlorinated dibenzo-p-dioxin and furan (PCDD/F) formation during municipal solid waste (MSW) incineration. Inorganic chlorine compounds were employed in this study to investigate their effects on PCDD/F formation through heterogeneous synthesis on fly ash surfaces. A fly ash sample obtained from a fluidized bed incinerator was sieved to different size fractions which served as the PCDD/F formation sources. The capability of different metal chlorides which facilitate the formation of PCDDs/Fs was found to follow the trends: Na 〈 Mg 〈 K 〈 AI 〈 Ca, when two particle fractions of 〉177 μm and 104-125 μm were used in the experiments. However, the capability of NaCI, MgCl2 and KCI did not seem much different from each other, whereas CaCl2 and AlCl3 were much more active in PCDD/F formation. NaCl and MgCl2 were relatively effective to produce more PCDDs, while KC1, AICl3 and CaCl2 generated more PCDFs during heterogeneous reactions occurring on fly ash. 2,3,7,8-TCDF was the most significant contributor to the toxicity of the PCDDs/Fs formed from inorganic chlorine sources. Decreasing the sizes of fly ash particles led to more active formation of PCDDs/Fs when NaCl was used as inorganic chlorine in the experiment. The highest PCDDs/Fs produced from particles with size 〈37 μm, while the lowest PCDDs/Fs produced from particles with size 〉177μm. The toxicity generally increased with decreasing size of the fly ash particles. The formation of PCDDs was mainly facilitated by the two size fractions, 104-125 μm and 〈37μm, while the formation of PCDFs was favored by the two other size fractions, 〉177 μm and 53-104 μm.
基金supported by the Natural Science Foundation of China(No.41103061)the Doctoral Fund Project of the Ministry of Education of China(No.20110141120015)the National Basic Research Programme(973)of China(No.2011CB707106)
文摘In January 2013, a long-lasting severe haze episode occurred in Northern and Central China; at its maximum, it covered a land area of approximately 1.4 million km2. In Wuhan, the largest city in Central China, this event was the most severe haze episode in the 21st century. Aerosol samples of submicron particles (PMI.o) were collected during the long-lasting haze episode at an urban site and a suburban site in Wuhan to investigate the ion characteristics of PMi.0 in this area. The mass concentrations of PM1.0 and its water-soluble inorganic ions (WSIIs) were almost at the same levels at two sites, which indicates that PM1.0 pollution occurs on a regional scale in Wuhao. WSIIs (Na^+, NH4^+, K^+, Mg^2+, Ca^2+, Cl^-, NO3 and SO2-) were the dominant chemical species and constituted up to 48.4% and 47.4% of PM1.0 at WD and TH, respectively. The concentrations of PM1.0 and WSIIs on haze days were approximately two times higher than on normal days. The ion balance calculations indicate that the particles were more acidic on haze days than on normal days. The results of the back trajectory analysis imply that the high concentrations of PM1.0 and its water-soluble inorganic ions may be caused by stagnant weather conditions in Wuhan.
基金supported by“Strategic Priority Research Program”of the Chinese Academy of Sciences(No.XDB05020201)the Beijing Natural Science Foundation(No.8142034)
文摘In this study, we performed a highly time-resolved chemical characterization of nonrefractory submicron particles(NR-PM_1) in Beijing by using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer(HR-ToF-AMS). The results showed the average NR-PM_1 mass concentration to be 56.4 ± 58.0 μg/m^3, with a peak at 307.4 μg/m^3. Due to the high frequency of biomass burning in autumn, submicron particles significantly increased in organic content, which accounted for 51% of NR-PM_1 on average. Secondary inorganic aerosols(sulfate + nitrate + ammonium) accounted for 46% of NR-PM_1, of which sulfate,nitrate, and ammonium contributed 15%, 20%, and 11%, respectively. To determine the intrinsic relationships between the organic and inorganic species, we used the positive matrix factorization(PMF) model to merge the high-resolution mass spectra of the organic species and NO+and NO_2~+ions. The PMF analysis separated the mixed organic and nitrate(NO+and NO_2~+) spectra into four organic factors, including hydrocarbon-like organic aerosol(HOA), oxygenated organic aerosol(OOA), cooking organic aerosol(COA), and biomass burning organic aerosol(BBOA), as well as one nitrate inorganic aerosol(NIA) factor. COA(33%) and OOA(30%) contributed the most to the total organic aerosol(OA) mass, followed by BBOA(20%) and HOA(17%). We successfully quantified the mass concentrations of the organic and inorganic nitrates by the NO+and NO2+ions signal in the organic and NIA factors. The organic nitrate mass varied from 0.01-6.8 μg/m^3, with an average of 1.0 ±1.1 μg/m^3, and organic nitrate components accounted for 10% of the total nitrate mass in this observation.