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Current and future hot-spots and hot-moments of nitrous oxide emission in a cold climate river basin
2018
Shrestha, Narayan Kumar | Wang, Junye
An ecosystem in a cold climate river basin is vulnerable to the effects of climate change affecting permafrost thaw and glacier retreat. We currently lack sufficient data and information if and how hydrological processes such as glacier retreat, snowmelt and freezing-thawing affect sediment and nutrient runoff and transport, as well as N₂O emissions in cold climate river basins. As such, we have implemented well-established, semi-empirical equations of nitrification and denitrification within the Soil and Water Assessment Tool (SWAT), which correlate the emissions with water, sediment and nutrients. We have tested this implementation to simulate emission dynamics at three sites on the Canadian prairies. We then regionalized the optimized parameters to a SWAT model of the Athabasca River Basin (ARB), Canada, calibrated and validated for streamflow, sediment and water quality. In the base period (1990–2005), agricultural areas (2662 gN/ha/yr) constituted emission hot-spots. The spring season in agricultural areas and summer season in forest areas, constituted emission hot-moments. We found that warmer conditions (+13% to +106%) would have a greater influence on emissions than wetter conditions (−19% to +13%), and that the combined effect of wetter and warmer conditions would be more offsetting than synergetic. Our results imply that the spatiotemporal variability of N₂O emissions will depend strongly on soil water changes caused by permafrost thaw. Early snow freshet leads to spatial variability of soil erosion and nutrient runoff, as well as increases of emissions in winter and decreases in spring. Our simulations suggest crop residue management may reduce emissions by 34%, but with the mixed results reported in the literature and the soil and hydrology problems associated with stover removal more research is necessary. This modelling tool can be used to refine bottom-up emission estimations at river basin scale, test plausible management scenarios, and assess climate change impacts including climate feedback.
Показать больше [+] Меньше [-]Baseline characterisation of source contributions to daily-integrated PM2.5 observations at Cape Grim using Radon-222
2018
Crawford, Jagoda | Chambers, Scott D. | Cohen, David D. | Williams, Alastair G. | Atanacio, Armand
We discuss 15 years (2000–2015) of daily-integrated PM₂.₅ samples from the Cape Grim Station. Ion beam analysis and positive matrix factorisation are used to identify six source-type fingerprints: fresh sea salt (57%); secondary sulfate (14%); smoke (13%); aged sea salt (12%); soil dust (2.4%); and industrial metals (1.5%). An existing hourly radon-only baseline selection technique is modified for use with the daily-integrated observations. Results were not significantly different for days on which >20 hours were below the baseline radon threshold compared with days when all 24 hours satisfied the baseline criteria. This relaxed daily baseline criteria increased the number of samples for analysis by almost a factor of two. Two radon baseline thresholds were tested: historic (100 mBq m⁻³), and revised (50 mBq m⁻³). Median aerosol concentrations were similar for both radon thresholds, but maximum values were higher for the 100 mBq m⁻³ threshold. Back trajectories indicated more interaction with southern Australia and the Antarctic coastline for air masses selected with the 100 mBq m⁻³ threshold. Radon-only baseline selection using the 50 mBq m⁻³ threshold was more selective of minimal terrestrial influence than a similar recent study using wind direction and back trajectories. The ratio of concentrations between terrestrial and baseline days for the primary sources soil, smoke and industrial metals was 3.4, 2.6, and 5.5, respectively. Seasonal cycles of soil dust had a summer maximum and winter minimum. Seasonal cycles of smoke were of similar amplitude for terrestrial and baseline events, but of completely different shape: peaking in autumn and spring for terrestrial events, compared to summer for baseline conditions. Seasonal cycles of industrial metals had a summer maximum and winter minimum. A significant fraction of the Cape Grim baseline smoke and industrial metal contributions appeared to be derived from long-term transport (>3 weeks since last terrestrial influence).
Показать больше [+] Меньше [-]Aqueous and organic extract of PM2.5 collected in different seasons and cities of Japan differently affect respiratory and immune systems
2018
Chowdhury, Pratiti Home | Okano, Hitoshi | Honda, Akiko | Kudou, Hitomi | Kitamura, Gaku | Ito, Sho | Ueda, Kayo | Takano, Hirohisa
Particulate matter with diameters <2.5 μm (i.e., PM₂.₅) has multiple natural and anthropological sources. The association between PM₂.₅ and the exacerbation of respiratory allergy and asthma has been well studied, but the components of PM₂.₅ that are responsible for allergies have not yet been determined. Here, we elucidated the effects of aqueous and organic extract of PM₂.₅ collected during four seasons in November 2014–December 2015 in two cities (Kawasaki, an industrial area and Fukuoka, an urban area affected by transboundary pollution matter) of Japan on respiratory health. Ambient PM₂.₅ was collected by high-volume air samplers and extracted into water soluble and lipid soluble components. Human airway epithelial cells, murine bone marrow-derived antigen-presenting cells (APC) and splenocytes were exposed to PM₂.₅ extracts. We measured the cell viability and release of interleukin (IL)-6 and IL-8 from airway epithelial cells, the DEC205 and CD86 expressions on APCs and cell proliferation, and TCR and CD19 expression on splenocytes. The water-soluble or aqueous extracts, especially those from Kawasaki in fall, had a greater cytotoxic effect than the lipid-soluble or organic extracts in airway epithelial cells, but they caused almost no pro-inflammatory response. Extract of fall, especially the aqueous extract from Fukuoka, increased the DEC205 and CD86 expressions on APC. Moreover, aqueous extracts of fall, summer, and spring from Fukuoka significantly increased proliferation of splenocytes. Organic extract of spring and summer from Kawasaki significantly elevated the TCR expression, and organic extract of summer from Kawasaki decreased the CD19 expression. These results suggest that PM₂.₅ extract samples are responsible for cytotoxicity in airway epithelial cells and for activating APCs and T-cells, which can contribute to the exacerbation of respiratory diseases such as asthma. These effects can differ by PM₂.₅ components, collection areas and seasons.
Показать больше [+] Меньше [-]Seasonal variabilities in chemical compounds and acidity of aerosol particles at urban site in the west Pacific
2018
Pan, Xiaole | Uno, Itsushi | Wang, Zhe | Yamamoto, Shigekazu | Hara, Yukari | Wang, Zifa
Mass concentrations of chemical compounds in both PM2.5 (particle aerodynamic diameter, Dp < 2.5 μm) and PM2.5-10 (2.5 < Dp < 10 μm), and acidity of aerosol particles were measured at an urban site in western Japan using a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-12) throughout 2014. Mass concentrations of both PM2.5 and sulfate had distinct seasonal variabilities with maxima in spring and winter, mostly due to long-range transport with the prevailing westerly wind. Mass concentration of nitrate in PM2.5 (fNO3) showed an obvious warm-season-low and cold-season-high pattern as a result of both gas-aerosol phase equilibrium processes under high temperature conditions as well as transport. Nitrate in PM2.5-10 (cNO3) increased during long-range transport of dust, implying the great importance of heterogeneous processes at the surface of coarse mode particles. In this study, Δ[H+] (derived from the difference in pH of extract liquid with/without sampling) was used to indicate the acidity of particles. We found that acidity of particles in PM2.5 (fΔH) was mostly positive with a maximum in August because of the large fraction of nitrate and sulfate. Acidity of particles in PM2.5-10 (cΔH) was negative in winter and spring due to presence of alkaline matter from crustal sources. This study highlights the great importance of anthropogenic pollutants on the acidity of particles in the western Pacific Ocean and further impact on the marine environment and climate.
Показать больше [+] Меньше [-]Nitrogen source track and associated isotopic dynamic characteristic in a complex ecosystem: A case study of a subtropical watershed, China
2018
Hao, Zhuo | Zhang, Xinyu | Gao, Yang | Xu, Zhiwei | Yang, Fengting | Wen, Xuefa | Wang, Yueming
By identifying the main sources of nitrate (NO3−) can obtain useful information to support the management of NO3− pollution, particularly in subtropical catchments with shallow drinking water wells. This study used water chemistry and dual stable isotopes δ15N and δ18O methods to assess seasonal and spatial variations of NO3− in precipitation, surface water, and groundwater in an agricultural and forest subtropical catchment in Jiangxi Province, China. The maximum concentrations of nitrate-nitrogen (NO3−-N) and ammonium-nitrogen (NH4+-N) were 10.4 and 10.8 mg L−1in samples collected from 221 rainfall events from 2011 to 2013. About 4.4% and 12.3% NH4+-N concentrations of surface water and groundwater exceeded the thresholds of 1.0 and 0.2 mg L−1. The NO3−-N concentrations in surface water were closely correlated with NH4+-N concentrations in surface water and groundwater (r = −0.71 and r = −0.71, P < 0.05). The concentrations of NH4+-N and NO3−-N were significantly higher in a fishery pond and nearby drinking wells than in other monitoring points. Annual exports of NO3−-N and NH4+-N were 4.06 × 104 and 8.14 × 103 kg yr−1, respectively and NO3−-N is the main form of N loss. The δ15N values ranged from 0‰ to 20‰ in surface water and groundwater, and the δ18O values ranged from 0‰ to 15‰ and 1‰–13‰, respectively. Dual stable isotope natural abundance distribution and water chemistry [NO3−]/[Cl−] molar ratio information suggested that manure and sewage and soil N were the main sources of NO3− in surface water and manure and sewage in groundwater in summer and winter. In spring, water occurred denitrification and ammonium fertilizer, manure and sewage were the main sources of NO3− in surface water and groundwater which sampling points were closer residential area and fish ponds than paddy field and local farmers used more Manure. Manure applications should be reasonable around drinking water wells to protect the drinking water quality.
Показать больше [+] Меньше [-]Improved rice residue burning emissions estimates: Accounting for practice-specific emission factors in air pollution assessments of Vietnam
2018
Lasko, Kristofer | Vadrevu, Krishna
In Southeast Asia and Vietnam, rice residues are routinely burned after the harvest to prepare fields for the next season. Specific to Vietnam, the two prevalent burning practices include: a). piling the residues after hand harvesting; b). burning the residues without piling, after machine harvesting. In this study, we synthesized field and laboratory studies from the literature on rice residue burning emission factors for PM2.5. We found significant differences in the resulting burning-practice specific emission factors, with 16.9 g kg−2(±6.9) for pile burning and 8.8 g kg−2(±3.5) for non-pile burning. We calculated burning-practice specific emissions based on rice area data, region-specific fuel-loading factors, combined emission factors, and estimates of burning from the literature. Our results for year 2015 estimate 180 Gg of PM2.5 result from the pile burning method and 130 Gg result from non-pile burning method, with the most-likely current emission scenario of 150 Gg PM2.5 emissions for Vietnam. For comparison purposes, we calculated emissions using generalized agricultural emission factors employed in global biomass burning studies. These results estimate 80 Gg PM2.5, which is only 44% of the pile burning-based estimates, suggesting underestimation in previous studies. We compare our emissions to an existing all-combustion sources inventory, results show emissions account for 14–18% of Vietnam's total PM2.5 depending on burning practice. Within the highly-urbanized and cloud-covered Hanoi Capital region (HCR), we use rice area from Sentinel-1A to derive spatially-explicit emissions and indirectly estimate residue burning dates. Results from HYSPLIT back-trajectory analysis stratified by season show autumn has most emission trajectories originating in the North, while spring has most originating in the South, suggesting the latter may have bigger impact on air quality. From these results, we highlight locations where emission mitigation efforts could be focused and suggest measures for pollutant mitigation. Our study demonstrates the need to account for emissions variation due to different burning practices.
Показать больше [+] Меньше [-]Using rush hour and daytime exposure indicators to estimate the short-term mortality effects of air pollution: A case study in the Sichuan Basin, China
2018
Guo, Bing | Chen, Fei | Deng, Ying | Zhang, Hongliang | Qiao, Xue | Qiao, Zhijiao | Ji, Kui | Zeng, Jing | Luo, Bin | Zhang, Wei | Zhang, Yuqin | Zhao, Xing
Daily mean concentrations of air pollutants have been widely used as exposure indicators to estimate the short-term mortality effects of outdoor air pollution. However, daily mean concentrations might insufficiently represent the true exposure level because of the diurnal variations of air pollutants and various human activity patterns. Daytime or rush-hour concentrations may lead to better estimations.Our study aimed to imitate the true exposure level under assumptions about human activity patterns and to examine the short-term mortality effects of the exposure to air pollution during a) the morning-evening rush hours (ME), b) the morning-lunch-evening rush hours (MLE), and c) the whole daytime (WDT) in Chengdu, Sichuan Basin, China.We investigated the diurnal variations of PM₂.₅, SO₂, and O₃ and examined the associations between the three pollutants and nonaccidental mortality, cardiovascular mortality, respiratory mortality using generalized additive model. Three novel exposure indicators (ME, MLE, and WDT) were employed to imitate the most probable exposure levels. Relative change of excess risk (ER) was used to compare effects estimated from models with different exposure indicators.In the relationship of PM₂.₅ and mortality, ERs estimated from the novel-indicator models decreased by 4.88%–11.89% in comparison with ERs from the daily-indicator models. All the three novel indicators of SO₂ offered lower ERs of respiratory mortality than the daily indicator did. Significant associations were observed in O₃-nonaccidental mortality at lag0 in both winter and spring, and O₃-cardiovascular mortality at lag0 in winter. Overall, majority of effect estimates based on rush-hour or daytime indicators were lower than the estimates based on daily mean concentrations.The use of daily mean concentrations may bias exposure assessment and thus inflating effect estimates. This study highlights the importance of rush-hour and daytime exposure and provides alternative indicators for estimating acute effects of air pollution.
Показать больше [+] Меньше [-]Occurrence and profile of organophosphorus compounds in fine and coarse particulate matter from two urban areas of China and Pakistan
2018
Faiz, Yasir | Siddique, Naila | He, Huan | Sun, Cheng | Waheed, Shahida
Seven organophosphorus compounds (OPs) were measured in urban fine and coarse particulate matter (PM) collected from two sites of Nanjing (XCNUC), China and Islamabad (APHSP), Pakistan. The fine PM mass at APHSP site was significantly higher (p = 0.005) in the spring (mean 22.5 μg/m³) than in the summer (mean 12.7 μg/m³). The total concentration, ∑⁷OPs, of samples collected at APHSP was found significantly higher in coarse (range 672–47621 pg/m³) than in fine PM (range 1200–15213 pg/m³); while ∑⁷OPs from XCNUC in fine (range 1696–15063 pg/m³) and coarse PM (range 2053–5379 pg/m³) were statistically different in samples during summer, based on two-sample t-test at 0.05 confidence interval. Seasonally, ∑⁷OPs was found to be higher in the samples of Nanjing (9510 ± 3633 pg/m³) in the summer than in the spring. In contrast, the samples of Islamabad had higher ∑⁷OPs (25558 ± 16255 pg/m³) in the spring than in the summer. Tri(chloropropyl) phosphate (TCEP) was found at higher concentration than any other OPs in the samples from the XCNUC site. Triphenyl phosphate (TPhP) was found at extremely high levels from APHSP, which may attributed to its use in jet fuel. Most of the ∑OPs concentrations were found significantly different in both PMs at both sites due to their diverse sources. Both sites showed strong correlation of ∑OPs with TCEP in both PMs, indicating similar mode of transfer from sources like plastics, lacquer, paint, glue, industrial processes and foam fillers. Relative abundance of OPs in fine and coarse PM differs amongst OP congeners and concerning seasons, with these variations attributed to different mechanisms of mass transfer such as volatilization, condensation and abrasions. Moreover, triphenylphosphine oxide (TPPO) has been reported in outdoor PMs. This is the first study on the occurrence of OPs in atmospheric fine and coarse PM and their seasonal variation from Pakistan and China.
Показать больше [+] Меньше [-]Characterizing benzene series (BTEX) pollutants build-up process on urban roads: Implication for the importance of temperature
2018
Liu, An | Hong, Nian | Zhu, Panfeng | Guan, Yuntao
Benzene series (BTEX) pollutants which are generated by traffic can deposit (build-up) on urban road surfaces. When they are washed-off by stormwater runoff, BTEX are toxic to ecological and human health if the stormwater is reused. To understand the risk posed by BTEX, it is essential to have an in-depth investigation on BTEX build-up, one of the most important stormwater pollutant processes. This study analysed the relationship between BTEX build-up and BTEX build-up's influential factors. The outcomes confirmed an important role of climatic factors (particularly temperature) on influencing BTEX build-up. This has not been considered in previous stormwater studies although this has been widely focused in atmospheric pollution. BTEX build-up loads were generally higher and the variability was low in dry seasons with low temperature such as winter and spring. Additionally, the influence of temperature on BTEX build-up on urban road surfaces is more important in the case of larger particles (such as >75 μm) than smaller particles. The study also showed that petrol station areas have a potential to export stormwater runoff with high BTEX concentrations, compared to typical urban roads. This is particularly applicable in winter and spring. These outcomes can provide useful guidance to improving stormwater quality modelling approaches, especially relevant to estimation of BTEX concentrations in the stormwater.
Показать больше [+] Меньше [-]The origin and migration of the dissolved sulfate from precipitation in Seoul, Korea
2018
Kim, Yeongmin | Lee, Insung | Lim, Chungwan | Farquhar, James | Lee, Sang-Mook | Kim, Hyoungbum
This study incorporated stable isotope analyses with chemical analyses to determine the origin and migration of sulfur sources in East Asia, and these findings were compared with our decadal research from 2000 to 2001 and 2002 to 2003. The multiple sulfur isotope composition (32S, 33S and 34S) of the dissolved sulfate in precipitation was first measured from 2011 to 2013 in Seoul, South Korea. The δ34Snss values were −1.1‰ to 7.9‰ (avg. 3.6‰), strongly suggesting that sulfur derived from the combustion of Chinese coal is the predominant source of sulfate in the Seoul region. Low NO3/SO42− ratios in the precipitation samples indicated an insignificant effect of sulfur from vehicle exhaust. The seasonal variation of δ34Snss values appears to be caused by increasing biogenic sulfur activity during the spring and summer seasons. The some Δ33S values (0.13‰–0.16‰) measured in the three samples were sufficiently small; thus, whether these values can be attributed to mass-independent fractionation remains unclear. Measuring the Δ33S anomalies in dissolved sulfate provides valuable insights for identifying the sources of sulfur transferred from the stratosphere to the troposphere and upper troposphere.
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