Combustion-derived substances in deep basins of Puget Sound: historical inputs from fossil fuel and biomass combustion

Reconstructions of 250 years historical inputs of two distinct types of black carbon (soot/graphitic black carbon (GBC) and char-BC) were conducted on sediment cores from two basins of the Puget Sound, WA. Signatures of polycyclic aromatic hydrocarbons (PAHs) were also used to support the historical reconstructions of BC to this system. Down-core maxima in GBC and combustion-derived PAHs occurred in the 1940s in the cores from the Puget Sound Main Basin, whereas in Hood Canal such peak was observed in the 1970s, showing basin-specific differences in inputs of combustion byproducts. This system showed relatively higher inputs from softwood combustion than the northeastern U.S. The historical variations in char-BC concentrations were consistent with shifts in climate indices, suggesting an influence of climate oscillations on wildfire events. Environmental loading of combustion byproducts thus appears as a complex function of urbanization, fuel usage, combustion technology, environmental policies, and climate conditions.     

Observations of hydroxyl and the sum of peroxy radicals at Summit,Greenland during summer 2003

The first measurements of peroxy (HO₂+RO₂) and hydroxyl (OH) radicals above the arctic snowpack were collected during the summer 2003 campaign at Summit, Greenland. The median measured number densities for peroxy and hydroxyl radicals were 2.2×10⁸ mol cm⁻³ and 6.4×10⁶ mol cm⁻³, respectively. The observed peroxy radical values are in excellent agreement ($R^2=0.83$, $\mathrm{M}/\mathrm{O}=1.06$) with highly constrained model predictions. However, calculated hydroxyl number densities are consistently more than a factor of 2 lower than the observed values. These results indicate that our current understanding of radical sources and sinks is in accord with our observations in this environment but that there may be a mechanism that is perturbing the (HO₂+RO₂)/OH ratio. This observed ratio was also found to depend on meteorological conditions especially during periods of high winds accompanied by blowing snow. Backward transport model simulations indicate that these periods of high winds were characterized by rapid transport (1–2 days) of marine boundary layer air to Summit. These data suggest that the boundary layer photochemistry at Summit may be periodically impacted by halogens.     

Concentrations and sources of carbonaceous aerosol in the atmosphere of Summit,Greenland

High-volume PM_2.5 samples were collected at Summit, Greenland for approximately six months from late May through December of 2006. Filters were composited and analyzed for source tracer compounds. The individual organic compounds measured at Summit are orders of magnitude smaller than concentrations measured at other sites, including locations representative of remote oceanic, and remote and urban continental aerosol. The measured tracers were used to quantify the contribution of biomass burning (0.6–0.9 ng C m^?3), vegetative detritus (0.3–0.9 ng C m^?3), and fossil fuel combustion (0.1–0.8 ng C m^?3) sources, 4% of OC total, to atmospheric organic carbon concentrations at the remote location of Summit, Greenland. The unapportioned organic carbon (96%) during the early summer period correlates well with the fraction of water soluble organic carbon, indicating secondary organic aerosol as a large source of organic carbon, supported by the active photochemistry occurring at Summit. To the author's knowledge, this paper represents the first source apportionment results for the polar free troposphere.     

Modeling the spectral optical properties of ammonium sulfate and biomass burning aerosols: parameterization of relative humidity effects and model results

The importance of including the global and regional radiative effects of aerosols in climate models has increasingly been realized. Accurate modeling of solar radiative forcing due to aerosols from anthropogenic sulfate and biomass burning emissions requires adequate spectral resolution and treatment of spatial and temporal variability. The variation of aerosol spectral optical properties with local relative humidity and dry aerosol composition must be considered. Because the cost of directly including Mie calculations within a climate model is prohibitive, parameterizations from off-line calculations must be used. Starting from a log-normal size distribution of dry ammonium sulfate, we developed optical properties for tropospheric sulfate aerosol at 15 relative humidities up to 99%. The resulting aerosol size distributions were then used to calculate bulk optical properties at wavelengths between 0.175 and 4 μm. Finally, functional fits of optical properties were made for each of 12 wavelength bands as a function of relative humidity. Significant variations in optical properties occurred across the total solar spectrum. Relative increases in specific extinction and asymmetry factor with increasing relative humidity became larger at longer wavelengths. Significant variation in single-scattering albedo was found only in the longest near-IR band. This is also the band with the lowest single scattering albedo. A similar treatment was done for aerosols from biomass burning. In this case, two size distributions were considered. One was based on a distribution measured for Northern Hemisphere temperate forest fires while the second was based on a measured size distribution for tropical fires. Equilibrium size distributions and compositions were calculated for 15 relative humidities and five black carbon fractions. Mie calculations and band averages of optical properties were done for each of the resulting 75 cases. Finally, fits were made for each of 12 spectral bands as functions of relative humidity and black carbon fraction. These optical properties result in global average forcing from anthropogenic sulfate aerosols of −0.81 Wm^-2. The global average forcing for biomass aerosols ranged from −0.23 to −0.25 Wm^-2 depending on the assumed size distribution, while fossil fuel organic and black carbon are estimated to heat the atmosphere by about 0.16 Wm^-2.     

Evaluation on estrogenicity and oxidative hepatotoxicity of fossil fuel industrial wastewater before and after the powdered activated carbon treatment

There are 10 manufacturers who produce fossil fuel products in the Da-Hse Industrial District, Kaohsiung County, southwestern Taiwan. Before discharging the wastewater into the nearby aquatic environment, the pretreated wastewater from these manufacturers must be processed in a treatment plant which includes four major processing units: equalization, a primary clarifier, an aeration basin, and a final clarifier. In order to estimate the potential environmental risks of industrial wastewater from each manufacturer and the treatment efficiency of the powdered activated carbon treatment (PACT) system used in this wastewater treatment plant, in vitro bioassays for estrogenicity and oxidative hepatotoxicity were carried out using a stably transfected human breast cancer cell line, MVLN, and a human hepatocellular carcinoma cell line, HepG2, respectively. Estrogenic substances occurred in nine of 10 pretreated wastewaters from these manufacturers in which the relative luciferase activity ranged from 18.9% to 98.0% for 1-fold-condensed wastewaters corresponding to the concentration of the original wastewater. The estrogenicity was highest at the influent of the treatment plant and decreased through the treatment process. About 81% estrogenicity clearance was found through all processing units. On the other hand, oxidative hepatotoxic substances existed in seven of 10 pretreated wastewaters from these manufacturers in which relative TBARs activity ranged from 18.5% to 43.0% for 1-fold-condensed wastewater. The TBARs of influent samples apparently decreased through the processing units until the aeration basin, but abruptly rose in the final clarifier, which was a result of the addition of an active charcoal-retrieving agent with the molecular formula of (C(2)H(3))(n)CONHCH(2)N(CH(3))(3)Cl and which had high TBARs activity. No TBARs activity being found in effluent samples could be a consequence of allowing sufficient time for coagulation between the active charcoal and its retrieval agent which decreased the residual active charcoal-retrieving agent. We concluded that the industrial wastewater treatment plant using the PACT system in the Da-Hse Industrial District is suitable for removing estrogenic substances and oxidative hepatotoxic substances discharged from these industrial manufacturers.     

A study of winter variability in carbon dioxide and Arctic haze aerosols at Barrow,Alaska

Relationships among atmospheric CO₂ concentration, excess sulfate and vanadium, and meteorological analyses for one winter at Barrow, Alaska were investigated. The results provided a basis for understanding the causes of short term CO₂ variability. The study indicated that peaks in CO₂ concentration were related to direct atmospheric transport of industrial pollutants from Eurasia. Evidence that background Arctic concentrations contained a pollution component was also found. Lowest CO₂ concentrations occurred with intrusions of Pacific air above the surface-based polluted Arctic air mass.     

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

The aerosol samples were collected from a high elevation mountain site, Nainital, in India (1958 m asl) during September 2006 to June 2007 and were analyzed for water-soluble inorganic species, total carbon, nitrogen, and their isotopic composition (δ¹³C and δ¹⁵N, respectively). The chemical and isotopic composition of aerosols revealed significant anthropogenic influence over this remote free-troposphere site. The amount of total carbon and nitrogen and their isotopic composition suggest a considerable contribution of biomass burning to the aerosols during winter. On the other hand, fossil fuel combustion sources are found to be dominant during summer. The carbon aerosol in winter is characterized by greater isotope ratios (av. ?24.0?‰), mostly originated from biomass burning of C₄ plants. On the contrary, the aerosols in summer showed smaller δ¹³C values (?26.0?‰), indicating that they are originated from vascular plants (mostly of C₃ plants). The secondary ions (i.e., SO₄ ^2?, NH₄ ⁺, and NO₃ ^?) were abundant due to the atmospheric reactions during long-range transport in both seasons. The water-soluble organic and inorganic compositions revealed that they are aged in winter but comparatively fresh in summer. This study validates that the pollutants generated from far distant sources could reach high altitudes over the Himalayan region under favorable meteorological conditions.     

The relationship between air pollution,fossil fuel energy consumption,and water resources in the panel of selected Asia-Pacific countries

The objective of the study is to examine the relationship between air pollution, fossil fuel energy consumption, water resources, and natural resource rents in the panel of selected Asia-Pacific countries, over a period of 1975–2012. The study includes number of variables in the model for robust analysis. The results of cross-sectional analysis show that there is a significant relationship between air pollution, energy consumption, and water productivity in the individual countries of Asia-Pacific. However, the results of each country vary according to the time invariant shocks. For this purpose, the study employed the panel least square technique which includes the panel least square regression, panel fixed effect regression, and panel two-stage least square regression. In general, all the panel tests indicate that there is a significant and positive relationship between air pollution, energy consumption, and water resources in the region. The fossil fuel energy consumption has a major dominating impact on the changes in the air pollution in the region.     

Chemical characterization of emissions from vegetable oil processing and their contribution to aerosol mass using the organic molecular markers approach

The organic fraction of aerosol emitted from a vegetable oil processing plant was studied to investigate the contribution of emissions to ambient particles in the surrounding area. Solvent-soluble particulate organic compounds emitted from the plant accounted for 10% of total suspended particles. This percentage was lower in the receptor sites (less than 6% of total aerosol mass). Nonpolar, moderate polar, polar, and acidic compounds were detected in both emitted and ambient aerosol samples. The processing and combustion of olive pits yielded a source with strong biogenic characteristics, such as the high values of the carbon preference index (CPI) for all compound classes. Polycyclic aromatic hydrocarbons (PAHs) detected in emissions were associated with both olive pits and diesel combustion. The chromatographic profile of dimethylphenanthrenes (DMPs) was characteristic of olive pit combustion. Organic aerosols collected in two receptor sites provided a different pattern. The significant contribution of vehicular emissions was identified by CPI values (approximately 1) of n-alkanes and the presence of the unresolved complex mixture (UCM). In addition, PAH concentration diagnostic ratios indicated that emissions from catalyst and noncatalyst automobiles and heavy trucks were significant. The strong even-to-odd predominance of n-alkanols, n-alkanoic acids, and their salts indicated the contribution of a source with biogenic characteristics. However, the profile of DMPs at receptor sites was similar to that observed for diesel particulates. These differences indicated that the contribution of vegetable oil processing emissions to the atmosphere was negligible.     

Hourly measurements of fine particulate sulfate and carbon aerosols at the Harvard-U.S. Environmental Protection Agency Supersite in Boston

Hourly concentrations of ambient fine particle sulfate and carbonaceous aerosols (elemental carbon [EC], organic carbon [OC], and black carbon [BC]) were measured at the Harvard-U.S. Environmental Protection Agency Supersite in Boston, MA, between January 2007 and October 2008. These hourly concentrations were compared with those made using integrated filter-based measurements over 6-day or 24-hr periods. For sulfate, the two measurement methods showed good agreement. Semicontinuous measurements of EC and OC also agreed (but not as well as for sulfate) with those obtained using 24-hr integrated filter-based and optical BC reference methods. During the study period, 24-hr PM2.5 (particulate matter [PM] < or = 2.5 microm in aerodynamic diameter) concentrations ranged from 1.4 to 37.6 microg/m3, with an average of 9.3 microg/m3. Sulfate as the equivalent of ammonium sulfate accounted for 39.1% of the PM2.5 mass, whereas EC and OC accounted for 4.2 and 35.2%, respectively. Hourly sulfate concentrations showed no distinct diurnal pattern, whereas hourly EC and BC concentrations peaked during the morning rush hour between 7:00 and 9:00 a.m. OC concentrations also exhibited nonpronounced, small peaks during the day, most likely related to traffic, secondary organic aerosol, and local sources, respectively.     

Characteristics of carbonaceous aerosols derived from long-term high-resolution measurements at a high-altitude site in the central Himalayas: radiative forcing estimates and role of meteorology and biomass burning

Environmental Science and Pollution Research - Simultaneous observations (2014–2017) of organic carbon (OC) and elemental carbon (EC) are made over a high-altitude site (Nainital,...     

Characterization and source presumption of wintertime submicron organic aerosols at Saitama,Japan, using the Aerodyne aerosol mass spectrometer

The chemical composition and size distribution of submicron aerosols were analyzed at a suburban site at Saitama, Japan, in the winter of 2004/2005, using an Aerodyne aerosol mass spectrometer. Although organics and nitrate were the dominant species during the sampling period, a large fraction of sulfate was observed at the accumulation mode when mass loading was low and wind speed was high. The size distributions of m/z 44 (mostly CO₂⁺) and sulfate aerosols during periods of high wind speed showed remarkable similarities in the accumulation mode, indicating that oxygenated organics were aged aerosols and internally mixed with sulfate. Ozone concentrations were also increased during these high wind speed periods although nighttime (e.g., 12/17 2004), indicating that the oxygenated compounds were strongly influenced by transported and aged air masses. The diurnal profiles of ultrafine-mode organics and hydrocarbon-like organic aerosols (HOA) were similar to NO_X derived from traffic and other combustion sources. The temporal variation of oxygenated organic aerosols (OOA) agreed well with that of nitrate as a secondary aerosol tracer, and the diurnal profile of the OOA fraction of organics increased during the day associated with higher UV light intensity. The result of time and size-resolved chemical composition of submicron particles indicated that the OOA is associated with both photochemical activity and transboundary pollution, and ultrafine-mode organic and HOA aerosols are mainly associated with combustion sources.     

Asymmetric investigation to track the effect of urbanization,energy utilization,fossil fuel energy and CO2 emission on economic efficiency in China: another outlook

Environmental Science and Pollution Research - The accelerated urbanization in China was already coupled with a steadily increasing demand for energy usage. The present study major aim was to...     

Heavy metals and Pb isotopic composition of aerosols in urban and suburban areas of Hong Kong and Guangzhou,South China—Evidence of the long-range transport of air contaminants

Rapid urbanization and industrialization in South China has placed great strain on the environment and on human health. In the present study, the total suspended particulate matter (TSP) in the urban and suburban areas of Hong Kong and Guangzhou, the two largest urban centres in South China, was sampled from December 2003 to January 2005. The samples were analysed for the concentrations of major elements (Al, Fe, Mg and Mn) and trace metals (Cd, Cr, Cu, Pb, V and Zn), and for Pb isotopic composition. Elevated concentrations of metals, especially Cd, Pb, V and Zn, were observed in the urban and suburban areas of Guangzhou, showing significant atmospheric trace element pollution. Distinct seasonal patterns were observed in the heavy metal concentrations of aerosols in Hong Kong, with higher metal concentrations during the winter monsoon period, and lower concentrations during summertime. The seasonal variations in the metal concentrations of the aerosols in Guangzhou were less distinct, suggesting the dominance of local sources of pollution around the city. The Pb isotopic composition in the aerosols of Hong Kong had higher ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios in winter, showing the influence of Pb from the northern inland areas of China and the Pearl River Delta (PRD) region, and lower ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios in summer, indicating the influence of Pb from the South Asian region and from marine sources. The back trajectory analysis showed that the enrichment of heavy metals in Hong Kong and Guangzhou was closely associated with the air mass from the north and northeast that originated from northern China, reflecting the long-range transport of heavy metal contaminants from the northern inland areas of China to the South China coast.     

Optical and thermal characteristics of carbonaceous aerosols measured at an urban site in Gwangju,Korea, in the winter of 2011

Carbonaceous components (organic carbon [OC] and elemental carbon [EC]) and optical properties (light absorption and scattering) of fine particulate matter (aerodynamic diameter <2.5 μm; PM_2.5) were simultaneously measured at an urban site in Gwangju, Korea, during the winter of 2011. OC was further classified into OC1, OC2, OC3, and OC4, based on a temperature protocol using a Sunset OC/EC analyzer. The average OC and EC concentrations were 5.0 ± 2.5 and 1.7 ± 0.9 μg C m^?3, respectively. The average single-scattering albedo (SSA) at a wavelength of 550 nm was 0.58 ± 0.11, suggesting that the aerosols observed in the winter of 2011 had a local warming effect in this area. During the whole sampling period, “stagnant PM” and “long-range transport PM” events were identified. The light absorption coefficient (b_abs) was higher during the stagnant PM event than during the long-range transport PM event due to the existence of abundant light-absorbing OC during the stagnant PM event. In particular, the OC2 and OC3 concentrations were higher during the stagnant PM event than those during the long-range transport event, suggesting that OC2 and OC3 might be more related to the light-absorbing OC. The light scattering coefficient (b_scat) was similar between the events. On average, the mass absorption efficiency attributed to EC (σ_EC) was 9.6 m² g^?1, whereas the efficiency attributed to OC (σ_OC) was 1.8 m² g^?1 at λ = 550 nm. Furthermore, the σ_EC is comparable among the PM event days, but the σ_OC for the stagnant PM event was significantly higher than that for the long-range transport PM event (1.7 vs. 0.5).

Implications: Optical and thermal properties of carbonaceous aerosol were measured at Gwangju, and carbonaceous aerosol concentration and optical property varied between “stagnant PM” and “long-range transport PM” events. More abundant light absorbing OC was observed during the stagnant PM event.     

Study of radioactive contamination in silts and aerosols at Aldama City,Mexico, due to the operation of a yellow-cake processing plant

The city of Aldama, Chihuahua, Mexico is located 30 km NNE of Chihuahua city. Three high-volume collectors with PM₁₀ heads were placed in specific locations in Aldama during the year 2011 to measure radioisotope concentrations in the air. The city area of 16 km² was divided into 64 squares of 500 × 500 m. At the vertices of the grid, silt samples were taken between January and June 2011, before the rains began. The concentrations of natural, cosmogenic, and anthropogenic radioactive isotopes were calculated in both filters and silts samples. The isotopes selected for the measurement were ²³⁸U, ²³²Th, ⁷Be, ¹³⁷Cs, and ⁴⁰K. Measurements of PM₁₀ and silts were performed during 2011, coinciding with the accident at Fukushima, Japan, on March 11. For this reason, we could see the ¹³⁷Cs in PM₁₀ increase between April and July; with the arrival of the rains, the ¹³⁷Cs concentration began to decrease in the air. The concentration of PM₁₀ measured by the equipment located at the Mexican Uranium plant (URAMEX, initials in Spanish) that was processing radioactive ores exceeded the standard values in February and March, when the air velocity increases. At City Hall, the concentration of PM₁₀ surpassed the value of the standard between May and July. This increased concentration is likely due to increased automobile traffic because City Hall is located in the city center. At a private home, the concentration of PM₁₀ surpassed the standard on several days during the year because the home is located on the outskirts of the city, where most of the streets are not paved. Due to the high concentrations of PM₁₀, especially at the collection point located at the private home, it is necessary to start taking steps to mitigate their spread before they cause health problems in the younger population and in older adults.

Implications: The radioisotope content found in the PM₁₀ confirms that the decision to place the Mexican Uranium plant (URAMEX, initials in Spanish) processing radioactive ores near the town of Aldama was not well thought out. Because the monitoring work was carried out in 2011 and coincided with the Fukushima accident, an increased concentration of ¹³⁷Cs could be detected in the PM₁₀. We made recommendations to the municipal authorities of the city to mitigate the concentration of particles in the air.