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Development of an on-line source-tagged model for sulfate, nitrate and ammonium: A modeling study for highly polluted periods in Shanghai, China
2017
Wu, Jian-Bin | Wang, Zifa | Wang, Qian | Li, Jie | Xu, Jianming | Chen, Huansheng | Ge, Baozhu | Zhou, Guangqiang | Chang, Luyu
An on-line source-tagged model coupled with an air quality model (Nested Air Quality Prediction Model System, NAQPMS) was applied to estimate source contributions of primary and secondary sulfate, nitrate and ammonium (SNA) during a representative winter period in Shanghai. This source-tagged model system could simultaneously track spatial and temporal sources of SNA, which were apportioned to their respective primary precursors in a simulation run. The results indicate that in the study period, local emissions in Shanghai accounted for over 20% of SNA contributions and that Jiangsu and Shandong were the two major non-local sources. In particular, non-local emissions had higher contributions during recorded pollution periods. This suggests that the transportation of pollutants plays a key role in air pollution in Shanghai. The temporal contributions show that the emissions from the “current day” (emission contribution from the current day during which the model was simulating) contributed 60%–70% of the sulfate and ammonium concentrations but only 10%–20% of the nitrate concentration, while the previous days’ contributions increased during the recorded pollution periods. Emissions that were released within three days contributed over 85% averagely for SNA in January 2013. To evaluate the source-tagged model system, the results were compared by sensitivity analysis (emission perturbation of −30%) and backward trajectory analysis. The consistency of the comparison results indicated that the source-tagged model system can track sources of SNA with reasonable accuracy.
Show more [+] Less [-]Below-cloud wet scavenging of soluble inorganic ions by rain in Beijing during the summer of 2014
2017
Xu, Danhui | Ge, Baozhu | Wang, Zifa | Sun, Yele | Chen, Yong | Ji, Dongshen | Yang, Ting | Ma, Zhiqiang | Cheng, Nianliang | Hao, Jianqi | Yao, Xuefeng
Wet deposition is one of the most important and efficient removal mechanisms in the reduction of air pollution. As a key parameter determining wet deposition, the wet scavenging coefficient (WSC) is widely used in chemical transport models (CTMs) and reported values have large uncertainties. In this study, a high-resolution observational dataset of the soluble inorganic aerosols (SO42−, NO3− and NH4+, hereafter SNA) in the air and in rainwater during multiple precipitation events was collected using sequential sampling and used to estimate the below-cloud WSC in Beijing during the summer of 2014. The average concentrations of SNA in precipitation during the observational period were 7.9 mg/L, 6.2 mg/L and 4.6 mg/L, with the contributions from below-cloud scavenging constituting 56%, 61% and 47% of this, respectively. The scavenging ratios of SNA (i.e., the ratio of the concentrations in rain to concentrations in the air) were used with the height of the cloud base and the precipitation intensity to estimate the WSC. The estimated WSC of SO42− is comparable to that reported elsewhere. The relationship between the below-cloud WSC and the precipitation intensity followed an exponential power distribution (K=aPb) for SNA. In contrast to previous studies, this study considers the differences between the chemical compositions of the SNA, with the highest WSC for NO3−, followed by those of SO42− and NH4+. Therefore, we recommend that CTMs include ion specific WSCs in the future.
Show more [+] Less [-]Source apportionment of PM2.5 in North India using source-oriented air quality models
2017
Guo, Hao | Kota, Sri Harsha | Sahu, Shovan Kumar | Hu, Jianlin | Ying, Qi | Gao, Aifang | Zhang, Hongliang
In recent years, severe pollution events were observed frequently in India especially at its capital, New Delhi. However, limited studies have been conducted to understand the sources to high pollutant concentrations for designing effective control strategies. In this work, source-oriented versions of the Community Multi-scale Air Quality (CMAQ) model with Emissions Database for Global Atmospheric Research (EDGAR) were applied to quantify the contributions of eight source types (energy, industry, residential, on-road, off-road, agriculture, open burning and dust) to fine particulate matter (PM2.5) and its components including primary PM (PPM) and secondary inorganic aerosol (SIA) i.e. sulfate, nitrate and ammonium ions, in Delhi and three surrounding cities, Chandigarh, Lucknow and Jaipur in 2015. PPM mass is dominated by industry and residential activities (>60%). Energy (∼39%) and industry (∼45%) sectors contribute significantly to PPM at south of Delhi, which reach a maximum of 200 μg/m³ during winter. Unlike PPM, SIA concentrations from different sources are more heterogeneous. High SIA concentrations (∼25 μg/m³) at south Delhi and central Uttar Pradesh were mainly attributed to energy, industry and residential sectors. Agriculture is more important for SIA than PPM and contributions of on-road and open burning to SIA are also higher than to PPM. Residential sector contributes highest to total PM2.5 (∼80 μg/m³), followed by industry (∼70 μg/m³) in North India. Energy and agriculture contribute ∼25 μg/m³ and ∼16 μg/m³ to total PM2.5, while SOA contributes <5 μg/m³. In Delhi, industry and residential activities contribute to 80% of total PM2.5.
Show more [+] Less [-]Nitrogen loss from anaerobic ammonium oxidation coupled to Iron(III) reduction in a riparian zone
2017
Ding, Bangjing | Li, Zhengkui | Qin, Yunbin
Anaerobic ammonium oxidation coupled to iron(III) reduction (termed Feammox) is a recently discovered pathway of nitrogen cycling. However, little is known about the pathways of N transformation via Feammox process in riparian zones. In this study, evidence for Feammox in riparian zones with or without vegetation cover was demonstrated using isotope tracing technique and high-throughput sequencing technology. The results showed that Feammox could occur in riparian zones, and demonstrated that N2 directly from Feammox was dominant Feammox pathway. The Feammox rates in vegetated soil samples was 0.32–0.37 mg N kg⁻¹ d⁻¹, which is higher than that in un-vegetated soil samples (0.20 mg N kg⁻¹ d⁻¹). Moreover, the growth of vegetation led to a 4.99–6.41% increase in the abundance of iron reducing bacteria (Anaeromyxobacter, Pseudomonas and Geobacter) and iron reducing bacteria play an essential role in Feammox process. An estimated loss of 23.7–43.9 kg N ha⁻¹ year⁻¹ was associated with Feammox in the examined riparian zone. Overall, the co-occurrence of ammonium oxidation and iron reduction suggest that Feammox can play an essential role in the pathway of nitrogen removal in riparian zones.
Show more [+] Less [-]Stable isotope analyses of precipitation nitrogen sources in Guiyang, southwestern China
2017
Liu, Xue-Yan | Xiao, Hong-Wei | Xiao, Hua-Yun | Song, Wei | Sun, Xin-Chao | Zheng, Xu-Dong | Liu, Cong-Qiang | Koba, Keisuke
To constrain sources of anthropogenic nitrogen (N) deposition is critical for effective reduction of reactive N emissions and better evaluation of N deposition effects. This study measured δ¹⁵N signatures of nitrate (NO3⁻), ammonium (NH4⁺) and total dissolved N (TDN) in precipitation at Guiyang, southwestern China and estimated contributions of dominant N sources using a Bayesian isotope mixing model. For NO3⁻, the contribution of non-fossil N oxides (NOx, mainly from biomass burning (24 ± 12%) and microbial N cycle (26 ± 5%)) equals that of fossil NOx, to which vehicle exhausts (31 ± 19%) contributed more than coal combustion (19 ± 9%). For NH4⁺, ammonia (NH3) from volatilization sources (mainly animal wastes (22 ± 12%) and fertilizers (22 ± 10%)) contributed less than NH3 from combustion sources (mainly biomass burning (17 ± 8%), vehicle exhausts (19 ± 11%) and coal combustions (19 ± 12%)). Dissolved organic N (DON) accounted for 41% in precipitation TDN deposition during the study period. Precipitation DON had higher δ¹⁵N values in cooler months (13.1‰) than in warmer months (−7.0‰), indicating the dominance of primary and secondary ON sources, respectively. These results newly underscored the importance of non-fossil NOx, fossil NH3 and organic N in precipitation N inputs of urban environments.
Show more [+] Less [-]Impacts of climate and management on water balance and nitrogen leaching from montane grassland soils of S-Germany
2017
Fu, Jin | Gasche, R. | Wang, Na | Lü, Haiyan | Butterbach-Bahl, Klaus | Kiese, Ralf
In this study water balance components as well as nitrogen and dissolved organic carbon leaching were quantified by means of large weighable grassland lysimeters at three sites (860, 770 and 600 m a.s.l.) for both intensive and extensive management. Our results show that at E600, the site with highest air temperature (8.6 °C) and lowest precipitation (981.9 mm), evapotranspiration losses were 100.7 mm higher as at the site (E860) with lowest mean annual air temperature (6.5 °C) and highest precipitation (1359.3 mm). Seepage water formation was substantially lower at E600 (−440.9 mm) as compared to E860. Compared to climate, impacts of management on water balance components were negligible. However, intensive management significantly increased total nitrogen leaching rates across sites as compared to extensive management from 2.6 kg N ha−1 year−1 (range: 0.5–6.0 kg N ha−1 year−1) to 4.8 kg N ha−1 year−1 (range: 0.9–12.9 kg N ha−1 year−1). N leaching losses were dominated by nitrate (64.7%) and less by ammonium (14.6%) and DON (20.7%). The low rates of N leaching (0.8–6.9% of total applied N) suggest a highly efficient nitrogen uptake by plants as measured by plant total N content at harvest. Moreover, plant uptake was often exceeding slurry application rates, suggesting further supply of N due to soil organic matter decomposition. The low risk of nitrate losses via leaching and surface runoff of cut grassland on non-sandy soils with vigorous grass growth may call for a careful site and region specific re-evaluation of fixed limits of N fertilization rates as defined by e.g. the German Fertilizer Ordinance following requirements set by the European Water Framework and Nitrates Directive.
Show more [+] Less [-]Inter-species and intra-annual variations of moss nitrogen utilization: Implications for nitrogen deposition assessment
2017
Dong, Yu-Ping | Liu, Xue-Yan | Sun, Xin-Chao | Song, Wei | Zheng, Xu-Dong | Li, Rui | Liu, Cong-Qiang
Moss nitrogen (N) concentrations and natural 15N abundance (δ15N values) have been widely employed to evaluate annual levels and major sources of atmospheric N deposition. However, different moss species and one-off sampling were often used among extant studies, it remains unclear whether moss N parameters differ with species and different samplings, which prevented more accurate assessment of N deposition via moss survey. Here concentrations, isotopic ratios of bulk carbon (C) and bulk N in natural epilithic mosses (Bryum argenteum, Eurohypnum leptothallum, Haplocladium microphyllum and Hypnum plumaeforme) were measured monthly from August 2006 to August 2007 at Guiyang, SW China. The H. plumaeforme had significantly (P < 0.05) lower bulk N concentrations and higher δ13C values than other species. Moss N concentrations were significantly (P < 0.05) lower in warmer months than in cooler months, while moss δ13C values exhibited an opposite pattern. The variance component analyses showed that different species contributed more variations of moss N concentrations and δ13C values than different samplings. Differently, δ15N values did not differ significantly between moss species, and its variance mainly reflected variations of assimilated N sources, with ammonium as the dominant contributor. These results unambiguously reveal the influence of inter-species and intra-annual variations of moss N utilization on N deposition assessment.
Show more [+] Less [-]Chemical analysis of particulate products of aged 1,3,5-trimethylbenzene secondary organic aerosol in the presence of ammonia
2017
Huang, Mingqiang | Xu, Jun | Cai, Shunyou | Liu, Xingqiang | Hu, Changjin | Gu, Xuejun | Zhao, Weixiong | Fang, Li | Zhang, Weijun
Ammonia (NH3) gas-aging of secondary organic aerosol (SOA) results in the formation of organonitrogen compound is an important class of brown carbon. The particulate products of aged 1,3,5-trimethylbenzene (135-TMB) SOA in the presence of NH3 were measured by UV–Vis spectrophotometer, attenuated total reflectance-Fourier transform infrared (ATR-FTIR), and aerosol laser time-of-flight mass spectrometer (ALTOFMS) in present study. Experimental results indicated that NH3 has significant promotion effect on 135-TMB SOA formation. Organic ammonium salts, such as ammonium methyl glyoxylate, ammonium 3,5-dimethylbenzoate, which are formed from NH3 reactions with gaseous organic acids were detected as the principal particulate products of NH3-aged 135-TMB SOA. 4-methyl-imidazole-2-acetaldehyde, 4-methyl- 1H-imidazole and other imidazole products via the heterogeneous reactions between NH3 and dialdehydes of 135-TMB SOA were newly measured. The formation of imidazole products suggests that some ambient particles contained organonitrogen compounds may be come from this mechanism. The results of this study may provide valuable information for discussing SOA aging mechanisms and new route for NH3 deposition.
Show more [+] Less [-]Induced tolerance in situ to chronically PAH exposed ammonium oxidizers
2017
Lindgren, J Fredrik | Hassellöv, Ida-Maja | Nyholm, Jenny Rattfelt | Östin, Anders | Dahllöf, Ingela
Sediment was sampled in the vicinity of a long-term source of Polycyclic Aromatic Hydrocarbons (PAHs) to evaluate whether tolerance can be induced in situ. Total PAH concentrations as well as the bioavailable PAHs were measured, and for nine PAHs the pore water concentration could be calculated. An induced tolerance in the ammonium oxidizing community was detected at the site with highest PAH concentration and tolerance was strongest, although not significantly, correlated to bioavailable alkylated PAHs. In addition, the tolerant microbial community showed a significant lower baseline capability for nitrification with an on average 35% reduction compared to the other sites. Meiofaunal community structure differed between all sites, and the difference was significantly correlated to bioavailable alkylated PAHs and PAH31 concentrations. The results suggest that in order to judge magnitude of long-term effects, the bioavailable fraction is to be preferred, and when possible as estimation of the freely dissolved concentration.
Show more [+] Less [-]Trends in wet precipitation, particulate, and gas-phase species in New York State
2017
Rattigan, O.V. | Civerolo, K.L. | Felton, H.D.
Here we characterized wet deposition National Atmospheric Deposition Program (NADP) species and Clean Air Status and Trends Network (CASTNET) dry deposited particle and gas species across New York over the last 2-3 decades. In addition measurements of NH3 from the Ammonia Monitoring Network (AMoN) were analyzed. In general decreasing annual trends are observed for wet deposition SO42− and NO3− species and dry deposited particle SO42−, NO3− and NH4+ as well as gas phase SO2 and HNO3 consistent with reductions in SO2 and NOx emissions. Wet deposited NH4+ however does not show consistent trends with most sites showing little trend across the region and an indication that levels at some sites maybe increasing. NH3 concentrations also appear to be increasing although the data record is only 8 years. Base cations, Ca2+ and Mg2+ show some decreases in the 1980s but concentrations are relatively uniform since the mid-1990s. Na+ and K+ show large year to year variations, by more than an order of magnitude for Na+ due to influence of marine air at a near coastal site. In general there was a balance between the sum of cations and the sum of anions earlier in the record but the tendency has been for a cation excess in the more recent 5–10 years. Understanding the deposition of reduced nitrogen species is likely to be of concern for the foreseeable future. Such data are important in understanding acidification recovery in response to emission controls.
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