[Show abstract][Hide abstract] ABSTRACT: Even after its being phased out in gasoline in the late 90s, lead (Pb) is still present at relatively high levels in the atmosphere of Beijing, China (0.10–0.18 μg m−3). Its origin is subject to debate as several distinct sources may contribute to the observed pollution levels. This study proposes to constrain the origin(s) of Pb and strontium (Sr) in aerosols, by coupling both Pb and Sr isotope systematics. The characterisation of the main pollution sources (road traffic, smelters, metal refining plants, coal combustion, cement factories, and soil erosion) shows that they can unambiguously be discriminated by the multi-isotope approach (206Pb/204Pb and 87Sr/86Sr). The study of total suspended particulates (TSP) and fine particles (PM2.5) from Beijing and its vicinity indicates that both size fractions are controlled by the same sources. Lead isotopes indicate that metal refining plants are the major source of atmospheric lead, followed by thermal power stations and other coal combustion processes. The role of this latter source is confirmed by the study of strontium isotopes. Occasionally, emissions from cement plants and/or input from soil alteration are isotopically detectable.
[Show abstract][Hide abstract] ABSTRACT: The occurrence and characteristics of 2,3,7,8-substituted polybrominated and polychlorinated dibenzo-p-dioxins and dibenzofurans (PBDD/F and PCDD/F) from various combustion and metallurgic industrial thermal processes were investigated. PBDD/F levels from metallurgic processes (TEQ) concentrations from 0.14 to 1.5 ng Nm(-3), mass concentrations from 0.56 to 5.8 ng Nm(-3)) were markedly higher than those from combustion processes (TEQ) concentrations from 0.010 to 0.054 ng Nm(-3), mass concentrations from 0.025 to 0.15 ng Nm(-3)). This indicated that metallurgic processes could be important sources of PBDD/F. Consequently, more attention should be paid to the metallurgical emission sources in addition to combustion of brominated flame retardants (BFRs) and related products. Specific isomeric patterns for PCDD/F from various industrial sources were highly consistent, while PBDD/F patterns were not. This revealed that PCDD/F might form through a common mechanism such as de novo synthesis mechanism, while PBDD/F might form by different mechanisms in thermal processes such as precursor mechanisms. Finally, an approach to identify the PBDD/F sources in ambient air by using the PBDD/F to PCDD/F ratio was developed.
[Show abstract][Hide abstract] ABSTRACT: Very little is known about mixed polybrominated/chlorinated dibenzo-p-dioxins and dibenzofurans (PBCDD/F) in industrial thermal processes. In this study, the occurrences and characteristics of PBCDD/F from various incineration and metallurgical processes were investigated. In addition, PBCDD/F analytical protocols based on HRGC/HRMS were developed and optimized. The sum of isomer group concentrations ranged from 1.7-3740 pmol Nm(-3) for PBCDF and 0.2-582 pmol Nm(-3) for PBCDD. For some metallurgical industries, the amounts of PBDD/F and PBCDD/F emitted were similar to or even higher than the amounts of PCDD/F. The sources of bromine and brominated-precursors in these processes should be evaluated. The PBCDD/F characteristics investigated included isomer group patterns, ratio of bromine and chlorine incorporated in PBCDD/F, and ratio of halogenated furans to dioxins. Lower brominated PBCDD/F were binomially distributed. But in some cases, the concentrations of higher brominated PBCDD/F were much higher than predicted from the binomial distribution. The formation mechanisms of PBDD/F, PBCDD/F, and PCDD/F in these processes were also evaluated.
[Show abstract][Hide abstract] ABSTRACT: Atmospheric aerosols were collected during the scientific expedition to Mt. Qomolangma (Everest) in May-June, 2005. The elemental concentrations of the aerosols were determined by inductively coupled plasma mass spectrometry. This yielded data for the concentration of 14 elements: Na, Mg, Al, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, and Pb. The mean elemental concentrations were generally comparable with those from central Asia and the Arctic, while much higher than those from Antarctic. Size, morphology, and chemical composition of 900 individual aerosol particles were determined by scanning electron microscopy and energy-dispersive X-ray microanalysis. Based on morphology and elemental composition, the particles were clustered into eight groups: soot (8%), tar ball (3%), alumosilicates/silica (55%), calcium sulfate (16%), Ca/Mg carbonate (2%), Fe/Ti-rich particles (3%), Pb-rich particles (1%), and biological particles (12%). The sampling site, located at 6,520 m in the Himalayas, is particularly remote and located at high altitude. Nonetheless, high aerosol enrichment factors for copper, chromium, lead, nickel, vanadium, and zinc all suggest the influence of long-range transported pollution, while enrichment in calcium and the presence of alumino-silicates in individual particle analyses indicates a distinct mineral dust influence. The backward air mass trajectories showed that the northwestern part of India may contribute to the atmospheric aerosol in the central high Himalayas.
Environmental Monitoring and Assessment 01/2009; 160(1-4):323-35. · 1.68 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: The total nitrogen (TN) and water-soluble nitrogenous ions were determined by using CHN Elemental Analyzer and ion chromatography method, respectively, from November 24, 1998 to February 12, 1999 in Beijing. The average concentrations of TN, NH(4) (+) and NO(3) (-) were 10.62 microg N m(-3), 6.67 microg m(-3) and 10.01 microg m(-3), respectively. The total inorganic nitrogen (IN) calculated from NH(4) (+) and NO(3) (-) was 7.45 microg N m(-3), accounting for 70% of TN, i.e., 30% of TN existed as organic nitrogen form (ON). The correlation between ON and other pollution tracers showed that, coal combustion, biomass burning, soil humic matter and secondary formation were the important sources of ON in particulate matter in Beijing.
Bulletin of Environmental Contamination and Toxicology 10/2008; 82(3):332-7. · 1.11 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Two series of size-selective aerosol samples, PM2.5 and PM10, were collected in Beijing from July 2002 to July 2003. The samples were analyzed for levoglucosan and related saccharidic compounds, organic and elemental carbon, and ionic species. Levoglucosan and related saccharidic compounds were mostly present in the fine size fraction. The contribution from biomass burning to the carbonaceous aerosol in Beijing was estimated; biomass burning was responsible for 18–38% of the PM2.5 organic carbon and for 14–32% of the PM10 organic carbon. The biomass burning marker levoglucosan was present all year round in Beijing. High levoglucosan concentrations in October and November were attributed to corn field burning and burning of fallen leaves, while the high level observed on 7 May 2003 was tracked back to a boreal forest fire more than 1000 km away in northeastern China. The biomass burning contribution to the Beijing aerosol is made up of two parts, a background component, which is due to biofuel burning all year round in the neighboring countryside households, and a superimposed component from seasonal crop burning events and wild fires.
[Show abstract][Hide abstract] ABSTRACT: Scanning electron microscopy–energy dispersive X-ray analysis (SEM–EDX) was used for the analysis of 2500 single particles in five atmospheric aerosol samples collected during the spring and summer of 2000 in Beijing, China. Mineral dust appeared to be the dominant particles during an Asian dust episode, while in other circumstances mineral dust and S-containing particles constituted the major particle components. During anthropogenic pollution episodes in the summer, a large abundance of S-containing particles featured the atmospheric aerosol. Chemical and size distribution characteristics are discussed for Ca–S, K–S and Ca–K–S particle classes. Formation of Ca–K–S and other S-containing particle classes with high abundance was closely related to meteorological conditions such as relative humidity and cloud coverage. Simple and composite sulfate particles with an elongated crystalline morphology were detected which appear to be indicative of aqueous phase oxidation, such as in-cloud processing for sulfate formation pathway.
[Show abstract][Hide abstract] ABSTRACT: Using Monte Carlo simulation, the geometric and matrix effects on intensity and intensity ratio measured by EPMA were investigated for both synthetic particles and biomass burning particles. Three particulate standards, KCl, K2SO4, KHSO4, were prepared and measured along with biomass burning particles. The modified CASINO program (University of Sherbrooke, Quebec, Canada) at the University of Antwerp, Belgium was used. The relative intensities obtained by the UA version of the CASINO program appear to be in line with those from experiments.The CASINO program and iterative procedures were applied to quantitatively determinate the atomic fraction of K, Cl and S in particulate standard and real samples. After correcting the geometric and matrix effects, the atomic fraction ratio of K to Cl in KCl sample was found to be 1.007±0.025, 0.996±0.013 and 1.011±0.019 for experiments with high voltages of 15, 20 and 25 keV, respectively. The same procedure was also applied to K2SO4 and KHSO4 standard particle sample. The atomic fraction ratio of K to S was 1.945±0.049 (25 keV) for K2SO4 and 1.014±0.072 (20 keV) for KHSO4. These ratios obtained are close to the theoretic values 1 or 2. Reasonable data were obtained for biomass burning particles, indicating that it is possible to perform chemical speciation.
[Show abstract][Hide abstract] ABSTRACT: Twelve filter samples were sampled monthly during a continuous 1-year campaign at a remote site, Nam Co in central Tibetan Plateau. The total aerosol concentrations ranged from 0.48 μg/m 3 to 36.11 μg/m 3 with the annual average of 6.74 μg/m 3 , reflecting a typical background level. The composition and morphology of atmospheric aerosols with size ranging from 0.5 to 10 μm were investigated using a scanning electron microscope coupled with energy dispersive X-ray analysis. Then aerosol particles were classified into 7 groups: soot, tar ball, aluminosilicates/quartz, calcium sulfate, Ca/Mg carbonate, Fe/Ti oxide, and biological particle. Aerosol optical properties from the sun photometer and the results obtained by SEM-EDX could support and verify each other, providing complementary information on aerosol characteristics at Nam Co. Two distinct types of air masses arriving at Nam Co correspond to different aerosol constituent, showing that the summer monsoon circulation may bring considerable pollution from South Asia, while the westerly flow dominated in winter is relative clean.