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Towards a better spatial quantification of nitrogen deposition: A case study for Czech forests
2016
Hůnová, Iva | Kurfürst, Pavel | Vlček, Ondřej | Stráník, Vojtěch | Stoklasová, Petra | Schovánková, Jana | Srbová, Daša
The quantification of atmospheric deposition flux is essential for assessment of its impact on ecosystems. We present an advanced approach for the estimation of the spatial pattern of atmospheric nitrogen deposition flux over the Czech forests, collating all available measured data and model results. The aim of the presented study is to provide an improved, more complete, more reliable and more realistic estimate of the spatial pattern of nitrogen deposition flux over one country. This has so far usually been based on measurements of ambient NOx concentrations as dry deposition proxy, and NH4+ and NO3− in precipitation as wet deposition proxy. For estimation of unmeasured species contributing to dry deposition, we used the CAMx Eulerian photochemical dispersion model, coupled with the Aladin regional numeric weather prediction model. The contribution of fog and dissolved organic nitrogen was estimated using a geostatistical data driven model. We prepared individual maps for particular components applying the most relevant approach and then merged all layers to obtain a final map representing the best estimate of nitrogen deposition over the Czech Republic. Final maps accounting for unmeasured species clearly indicate that the approach used so far may result in a substantial underestimation of nitrogen deposition flux. Our results showed that nitrogen deposition over the Czech forested area in 2008 was well above 2 g N m−2 yr−1, with almost 70% of forested area receiving 3–4 g N m−2 yr−1. NH3 and gaseous HNO3, contributing about 80%, dominated the dry nitrogen deposition. Estimating the unmeasured nitrogen species by modeled values provides realistic approximations of total nitrogen deposition that also result in more realistic spatial patterns that could be used as input for further studies of likely nitrogen impacts on ecosystems.
Show more [+] Less [-]Chemical composition and source apportionment of size fractionated particulate matter in Cleveland, Ohio, USA
2016
Kim, Yŏng-ho | Krantz, Q Todd | McGee, John | Kovalcik, Kasey D. | Duvall, Rachelle M. | Willis, Robert D. | Kamal, Ali S. | Landis, Matthew S. | Norris, Gary A. | Gilmour, M Ian
The Cleveland airshed comprises a complex mixture of industrial source emissions that contribute to periods of non-attainment for fine particulate matter (PM2.5) and are associated with increased adverse health outcomes in the exposed population. Specific PM sources responsible for health effects however are not fully understood. Size-fractionated PM (coarse, fine, and ultrafine) samples were collected using a ChemVol sampler at an urban site (G.T. Craig (GTC)) and rural site (Chippewa Lake (CLM)) from July 2009 to June 2010, and then chemically analyzed. The resulting speciated PM data were apportioned by EPA positive matrix factorization to identify emission sources for each size fraction and location. For comparisons with the ChemVol results, PM samples were also collected with sequential dichotomous and passive samplers, and evaluated for source contributions to each sampling site. The ChemVol results showed that annual average concentrations of PM, elemental carbon, and inorganic elements in the coarse fraction at GTC were ∼2, ∼7, and ∼3 times higher than those at CLM, respectively, while the smaller size fractions at both sites showed similar annual average concentrations. Seasonal variations of secondary aerosols (e.g., high NO3− level in winter and high SO42− level in summer) were observed at both sites. Source apportionment results demonstrated that the PM samples at GTC and CLM were enriched with local industrial sources (e.g., steel plant and coal-fired power plant) but their contributions were influenced by meteorological conditions and the emission source's operation conditions. Taken together the year-long PM collection and data analysis provides valuable insights into the characteristics and sources of PM impacting the Cleveland airshed in both the urban center and the rural upwind background locations. These data will be used to classify the PM samples for toxicology studies to determine which PM sources, species, and size fractions are of greatest health concern.
Show more [+] Less [-]Characterization and source apportionment of size-segregated atmospheric particulate matter collected at ground level and from the urban canopy in Tianjin
2016
Wang, Jiao | Zhou, Ming | Liu, Bao-shuang | Wu, Jian-hui | Peng, Xing | Zhang, Yu-fen | Han, Su-qin | Feng, Yin-chang | Zhu, Tan
To investigate the size distributions of chemical compositions and sources of particulate matter (PM) at ground level and from the urban canopy, a study was conducted on a 255 m meteorological tower in Tianjin from December 2013 to January 2014. Thirteen sets of 8 size-segregated particles were collected with cascade impactor at 10 m and 220 m. Twelve components of particles, including water-soluble inorganic ions and carbonaceous species, were analyzed and used to apportion the sources of PM with positive matrix factorization. Our results indicated that the concentrations, size distributions of chemical compositions and sources of PM at the urban canopy were affected by regional transport due to a stable layer approximately 200 m and higher wind speed at 220 m. The concentrations of PM, Cl− and elemental carbon (EC) in fine particles at 10 m were higher than that at 220 m, while the reverse was true for NO3− and SO42−. The concentrations of Na+, Ca2+, Mg2+, Cl− and EC in coarse particles at 10 m were higher than that at 220 m. The size distributions of major primary species, such as Cl−, Na+, Ca2+, Mg2+ and EC, were similar at two different heights, indicating that there were common and dominant sources. The peaks of SO42−, NH4+, NO3− and organic carbon (OC), which were partly secondary generated species, shifted slightly to the smaller particles at 220 m, indicating that there was a different formation mechanism. Industrial pollution and coal combustion, re-suspended dust and marine salt, traffic emissions and transport, and secondary inorganic aerosols were the major sources of PM at both heights. With the increase in vertical height, the influence of traffic emissions, re-suspended dust and biomass burning on PM weakened, but the characteristics of regional transport from Hebei Province and Beijing gradually become obvious.
Show more [+] Less [-]Fine particulate matter (PM2.5) in Edmonton, Canada: Source apportionment and potential risk for human health
2016
Bari, Md Aynul | Kindzierski, Warren B.
To design effective PM2.5 control strategies in urban centers, there is a need to better understand local and remote sources influencing PM2.5 levels and associated risk to public health. An investigation of PM2.5 levels, sources and potential human health risk associated with trace elements in the PM2.5 was undertaken in Edmonton over a 6-year period (September 2009–August 2015). The geometric mean PM2.5 concentration of was 7.11 μg/m3 (interquartile range, IQR = 4.83–10.08 μg/m3). Positive matrix factorization (PMF) receptor modeling identified secondary organic aerosol (SOA) as the major contributor (2.2 μg/m3, 27%), followed by secondary nitrate (1.3 μg/m3, 17%) and secondary sulfate (1.2 μg/m3, 15%). Other local sources included transportation (1.1 μg/m3, 14%) and industry-related emissions (0.26 μg/m3, 3.4%), biomass burning (1.0 μg/m3, 13%) and soil (0.54 μg/m3, 6.8%). Five factors (i.e., SOA, secondary nitrate, secondary sulfate, transportation and biomass burning) contributed more than 85% to PM2.5 for the 2009–2015 period. Geometric (arithmetic) mean and maximum ambient air concentrations for hazardous trace elements of public health concern in PM2.5 during the study period were below United States regulatory agency chronic and acute health risk screening criteria. Carcinogenic and non-carcinogenic risk of trace elements and source-specific risk values were well below acceptable and safe levels of risks recommended by regulatory agencies. More work is needed to understand the origin of potential SOA and wintertime wood burning sources in Edmonton and the surrounding region and to apply source-risk apportionment using all available hazardous air pollutants (HAPs) including organic compounds to better interpret the potential health risk posed by various sources in urban areas.
Show more [+] Less [-]Evolution of secondary inorganic and organic aerosols during transport: A case study at a regional receptor site
2016
Peng, Jianfei | Hu, Min | Gong, Zhaoheng | Tian, Xudong | Wang, Ming | Zheng, Jing | Guo, Qingfeng | Cao, Wei | Lv, Wei | Hu, Weiwei | Wu, Zhijun | Guo, Song
Understanding the evolution of aerosols in the atmosphere is of great importance for improving air quality and reducing aerosol-related uncertainties in global climate simulations. Here, a unique haze episode at a regional receptor site near the East China Sea was examined as a case study of the aging process of atmospheric aerosols during transport. An increase in photochemical age from 5 h to more than 25 h and a progressive increase in the fitted mean particle diameter from 70 nm to approximately 300 nm were observed. According to the pollution features and meteorology conditions involved, pollution accumulation (PA), sea breeze (SB), and land breeze (LB) periods were identified. Concentrations of black carbon (BC), hydrocarbon-like organic aerosols (HOA), semi-volatile oxidized organic aerosols (SV-OOA), and nitrate increased by 7-fold up to 39-fold when the air masses passed through Taizhou, a nearby city. In addition, nitrate and SV-OOA dominated the aerosol composition in the urban outflow plumes (52% and 18%, respectively), yet they gradually decreased in concentration during transport. In contrast, sulfate and the low-volatile oxidized organic aerosols (LV-OOA) exhibited more regional footprints and potentially have similar formation mechanisms. The atomic oxygen-to-carbon (O/C) ratio also increased from 0.45 to 0.9, thereby suggesting that rapid formation of highly oxidized secondary organic aerosols (SOA) occurred during transport. Overall, these results provide valuable insight into the evolution of the chemical and physical features of aerosol pollution during transport and also highlight the need for regulatory controls of nitrogen oxides, sulfur dioxide, and VOCs to improve air quality on different scales.
Show more [+] Less [-]Light absorption enhancement of black carbon from urban haze in Northern China winter
2016
Chen, Bing | Bai, Zhe | Cui, Xinjuan | Chen, Jianmin | Andersson, August | Gustafsson, Örjan
Atmospheric black carbon (BC) is an important pollutant for both air quality and Earth's energy balance. Estimates of BC climate forcing remain highly uncertain, e.g., due to the mixing with non-absorbing components. Non-absorbing aerosols create a coating on BC and may thereby act as a lens which may enhance the light absorption. However, this absorption enhancement is poorly constrained. To this end a two-step solvent dissolution protocol was employed to remove both organic and inorganic coatings, and then investigate their effects on BC light absorption. Samples were collected at a severely polluted urban area, Jinan, in the North China Plain (NCP) during February 2014. The BC mass absorption cross-section (MAC) was measured for the aerosol samples before and after the solvent-decoating treatment, and the enhancement of MAC (EMAC) from the coating effect was defined as the ratio. A distinct diurnal pattern for the enhancement was observed, with EMAC 1.3 ± 0.3 (1 S.D.) in the morning, increasing to 2.2 ± 1.0 in the afternoon, after that dropping to 1.5 ± 0.8 in the evening-night. The BC absorption enhancement primarily was associated with urban-scale photochemical production of nitrate and sulfate aerosols. In addition to that, regional-scale haze plume with increasing sulfate levels strengthened the absorption enhancement. These observations offer direct evidence for an increased absorption enhancement of BC due to severe air pollution in China.
Show more [+] Less [-]Health risk assessment for exposure to nitrate in drinking water from village wells in Semarang, Indonesia
2016
Sadler, Ross | Maetam, Brooke | Edokpolo, Benjamin | Connell, Des | Yu, Jimmy | Stewart, Donald | Park, M.-J. | Gray, Darren | Laksono, Budi
The levels of nitrate in 52 drinking water wells in rural Central Java, Indonesia were evaluated in April 2014, and the results were used for a health risk assessment for the local populations by using probabilistic techniques. The concentrations of nitrate in drinking water had a range of 0.01–84 mg/L, a mean of 20 mg/L and a medium of 14 mg/L. Only two of the 52 samples exceeded the WHO guideline values of 50 mg/L for infant methaemoglobinaemia. The hazard quotient values as evaluated against the WHO guideline value at the 50 and 95 percentile points were HQ50 at 0.42 and HQ95 at 1.2, respectively. These indicated a low risk of infant methaemoglobinaemia for the whole population, but some risk for the sensitive portion of the population. The HQ50 and HQ95 values based on WHO acceptable daily intake dose for adult male and female were 0.35 and 1.0, respectively, indicating a generally a low level of risk. A risk characterisation linking birth defects to nitrate levels in water consumed during the first three months of pregnancy resulted in a HQ50/50 values of 1.5 and a HQ95/5 value of 65. These HQ values indicated an elevated risk for birth defects, in particular for the more sensitive population. A sanitation improvement program in the study area had a positive effect in reducing nitrate levels in wells and the corresponding risk for public health. For example, the birth defect HQ50/50 values for a subset of wells surveyed in both 2014 and 2015 was reduced from 1.1 to 0.71.
Show more [+] Less [-]Ambient concentration and dry deposition of major inorganic nitrogen species at two urban sites in Sichuan Basin, China
2016
Wang, Huanbo | Yang, Fumo | Shi, Guangming | Tian, Mi | Zhang, Leiming | Zhang, Liuyi | Fu, Chuan
To assess pollution levels of major inorganic nitrogen species and their atmospheric deposition input to sensitive ecosystems in Sichuan Basin, southwest China, ambient concentrations of oxidized (NOy ∼ NO2, HNO3, NO3−) and reduced (NHx = NH3, NH4+) nitrogen species were collected at two urban sites during four one-month periods, each in a different season from July 2014 to April 2015. Estimated annual mean concentration of NOy was 20.3 and 13.5 μg N m−3 in Chengdu and Wanzhou, respectively, and NHx was 16.9 and 13.6 μg N m−3, respectively. Back trajectory cluster analysis indicated that high levels of NOy and NHx in Chengdu were mainly caused by local emissions while those in Wanzhou were caused by both the local emissions and long-range transport of pollutants. On annual basis, NO2 contributed the most to NOy, followed by NO3− and HNO3, accounting for 87.5%, 10.5% and 2.0%, respectively, of NOy in Chengdu, and 91.4%, 6.9% and 1.7%, respectively, in Wanzhou. NH3 was the predominant contributor to NHx, contributing 65.6% and 72.2% in Chengdu and Wanzhou, respectively. Dry deposition fluxes were estimated using the inferential method with measured ambient concentrations and modelled dry deposition velocities. The total inorganic nitrogen dry deposition flux was estimated to be 21.4 and 8.5 kg N ha−1 yr−1, with 44.3% and 41.4% from NOy in Chengdu and Wanzhou, respectively. NO2 and NH3 each contributed about 80% of NOy and NHx dry deposition, respectively. Wet deposition was only collected in Wanzhou, where the annual wet deposition of NO3− and NH4+ was 4.5 and 15.7 kg N ha−1 yr−1, respectively. The total wet plus dry deposition was 28.7 kg N ha−1 yr−1 in Wanzhou with 72.2% from reduced nitrogen. Therefore, controlling NH3 emissions from agricultural, traffic, waste containers and sewage system sources would be effective to reduce the total nitrogen deposition in the Sichuan Basin area.
Show more [+] Less [-]Atmospheric S and N deposition relates to increasing riverine transport of S and N in southwest China: Implications for soil acidification
2016
Duan, Lei | Chen, Xiao | Ma, Xiaoxiao | Zhao, Bin | Larssen, Thorjørn | Wang, Shuxiao | Ye, Zhixiang
Following Europe and North America, East Asia has become a global hotspot for acid deposition, with very high deposition of both sulfur (S) and nitrogen (N) occurring in large areas of southwest and southeast China. This study shows that the outflow flux of sulfate (SO42−) in three major tributaries of the Upper Yangtze River in the Sichuan Basin in southwest China has been increasing over the last three decades, which implies the regional soil acidification caused by increasing sulfur dioxide (SO2) emissions. Since 2005, the outflow of SO42− to the Upper Yangtze River from the Sichuan Basin has even reached the atmospheric SO2 emission from the basin. In contrast to S emissions, the rapid increase in nitrogen (N) emissions, including nitrogen oxides (NOx) and ammonia (NH3), have resulted in only a slight increase in nitrate (NO3−) concentrations in surface waters, indicating a large retention of N in the basin. Although N deposition currently contributes much less than S to soil acidification in this area, it is possible that catchments receiving a high input of N may be unable to retain a large fraction of the N deposition over long periods.
Show more [+] Less [-]Deep challenges for China's war on water pollution
2016
Han, Dongmei | Currell, Matthew J. | Cao, Guoliang
China's Central government has released an ambitious plan to tackle the nation's water pollution crisis. However, this is inhibited by a lack of data, particularly for groundwater. We compiled and analyzed water quality classification data from publicly available government sources, further revealing the scale and extent of the crisis. We also compiled nitrate data in shallow and deep groundwater from a range of literature sources, covering 52 of China's groundwater systems; the most comprehensive national-scale assessment yet. Nitrate pollution at levels exceeding the US EPA's maximum contaminant level (10 mg/L NO3N) occurs at the 90th percentile in 25 of 36 shallow aquifers and 10 out of 37 deep or karst aquifers. Isotopic compositions of groundwater nitrate (δ15N and δ18ONO3 values ranging from −14.9‰ to 35.5‰ and −8.1‰ to 51.0‰, respectively) indicate many nitrate sources including soil nitrogen, agricultural fertilizers, untreated wastewater and/or manure, and locally show evidence of de-nitrification. From these data, it is clear that contaminated groundwater is ubiquitous in deep aquifers as well as shallow groundwater (and surface water). Deep aquifers contain water recharged tens of thousands of years before present, long before widespread anthropogenic nitrate contamination. This groundwater has therefore likely been contaminated due to rapid bypass flow along wells or other conduits. Addressing the issue of well condition is urgently needed to stop further pollution of China's deep aquifers, which are some of China's most important drinking water sources. China's new 10-point Water Pollution Plan addresses previous shortcomings, however, control and remediation of deep groundwater pollution will take decades of sustained effort.
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