scholarly journals MICS-Asia III: Multi-model comparison of reactive Nitrogen deposition over China

Author(s):  
Baozhu Ge ◽  
Syuichi Itahashi ◽  
Keiichi Sato ◽  
Danhui Xu ◽  
Junhua Wang ◽  
...  

Abstract. Atmospheric nitrogen deposition in China has attracted huge public attention in recently years due to the increasing anthropogenic emission of reactive nitrogen (Nr) and its impacts on the terrestrial and aquatic ecosystems. However, limited long-term and multi-site measurements have restrained the understanding on the mechanism of the Nr deposition as well as the chemical transport model (CTM) improvement. In this study, the performance of the simulated wet and dry deposition for different Nr species, i.e., particulate NO3− and NH4+, gaseous NOx, HNO3 and NH3, have been conducted using the framework of Model Inter-Comparison Study for Asia (MICS-Asia) phase III. Nine Models, including 5 WRF-CAMQ models, 2 self-developed regional models, a global model and a RAMS-CMAQ model, have been selected for the comparison. For wet depositions, observation data from 83 measurement sites of EANET, CREN, CAUDN, NADMN and DEE of China have been collected and normalized to compare with model results. In general, most models showed the consistent spatial and temporal variation of both oxidized N (Nox) and reduced N (Nrd) wet depositions in China with the NME around at 50 %, which is lower than the value of 70 % based on EANET observation over Asia. Both the ratio of wet or dry deposition to the total inorganic N deposition (TIN) and the ratios of TIN to their emissions have shown the consistent results with the NNDMN estimations. The performance of ensemble results (ENM) was further assessed with the measurement from satellite. In different regions of China, the results showed that the simulated Nox wet deposition was overestimated in North East China (NE) but underestimated in south of China (SE+SW), while the Nrd wet deposition was underpredicted in all regions by all models. The deposition of Nox have large uncertainties than the Nrd especially in North China (NC), indicating chemical reaction process is one of the most importance factors that affecting the model performance. Compared to Critical load (CL) value, the Nr deposition in NC, SE and SW reached or exceeded the reported CL value and exerted serious ecological impacts. The control of Nrd in NC and SW and Nox in SE would be effective to mitigate the TIN deposition in these regions. More interestingly, the Nr deposition in Tibet plateau with the high ratio of TIN/emission (~3.0), indicating a significant import from outside should be focused in the future due to its climatical influence to the sensitive ecosystem in whole China.

2020 ◽  
Vol 20 (17) ◽  
pp. 10587-10610
Author(s):  
Baozhu Ge ◽  
Syuichi Itahashi ◽  
Keiichi Sato ◽  
Danhui Xu ◽  
Junhua Wang ◽  
...  

Abstract. Atmospheric nitrogen deposition in China has attracted public attention in recent years due to the increasing anthropogenic emission of reactive nitrogen (Nr) and its impacts on the terrestrial and aquatic ecosystems. However, limited long-term and multisite measurements have restrained the understanding of the mechanism of the Nr deposition and the chemical transport model (CTM) improvement. In this study, the performance of the simulated wet and dry deposition for different Nr species, i.e., particulate NO3- and NH4+, gaseous NOx, HNO3 and NH3 have been conducted using the framework of Model Inter-Comparison Study for Asia (MICS-Asia) phase III. A total of nine models, including five Weather Research and Forecasting models coupled with the Community Multiscale Air Quality (WRF-CMAQ) models, two self-developed regional models, a global model and a Regional Atmospheric Modeling System coupled with the Community Multiscale Air Quality (RAMS-CMAQ) model have been selected for the comparison. For wet deposition, observation data from 83 measurement sites from the East Asia Acid Deposition Monitoring Network (EANET), Chinese Ecosystem Research Network (CERN), China Agricultural University Deposition Network (CAUDN), National Acid Deposition Monitoring Network (NADMN) and Department of Ecological Environment (DEE) of China have been collected and normalized for comparison with model results. In general, most models show the consistent spatial and temporal variation of both oxidized N (Nox) and reduced N (Nrd) wet deposition in China, with the normalized mean error (NME) at around 50 %, which is lower than the value of 70 % based on EANET observation over Asia. Both the ratio of wet or dry deposition to the total inorganic N (TIN) deposition and the ratios of TIN to their emissions have shown consistent results with the Nationwide Nitrogen Deposition Monitoring Network (NNDMN) estimates. The performance of ensemble results (ENMs) was further assessed with satellite measurements. In different regions of China, the results show that the simulated Nox wet deposition was overestimated in northeastern China (NE) but underestimated in the south of China, namely southeastern (SE) and southwestern (SW) China, while the Nrd wet deposition was underestimated in all regions by all models. The deposition of Nox has larger uncertainties than the Nrd, especially in northern China (NC), indicating the chemical reaction process is one of the most important factors affecting the model performance. Compared to the critical load (CL) value, the Nr deposition in NC, SE and SW reached or exceeded reported CL values and resulted in serious ecological impacts. The control of Nrd in NC and SW and Nox in SE would be an effective mitigation measure for TIN deposition in these regions. The Nr deposition in the Tibetan Plateau (TP) with a high ratio of TIN ∕ emission (∼3.0), indicates a significant transmission from outside. Efforts to reduce these transmissions ought to be paramount due the climatic importance of the Tibetan region to the sensitive ecosystems throughout China.


2019 ◽  
Vol 19 (24) ◽  
pp. 15587-15608 ◽  
Author(s):  
Lei Zhang ◽  
Peisheng Zhou ◽  
Shuzhen Cao ◽  
Yu Zhao

Abstract. One of the most important processes in the global mercury (Hg) biogeochemical cycling is the deposition of atmospheric Hg, including gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM), to the land surfaces. Results of wet, dry, and forest Hg deposition from global observation networks, individual monitoring studies, and observation-based simulations have been reviewed in this study. Uncertainties in the observation and simulation of global speciated atmospheric Hg deposition to the land surfaces have been systemically estimated based on assessment of commonly used observation methods, campaign results for comparison of different methods, model evaluation with observation data, and sensitivity analysis for model parameterization. The uncertainties of GOM and PBM dry deposition measurements come from the interference of unwanted Hg forms or incomplete capture of targeted Hg forms, while that of GEM dry deposition observation originates from the lack of a standardized experimental system and operating procedure. The large biases in the measurements of GOM and PBM concentrations and the high sensitivities of key parameters in resistance models lead to high uncertainties in GOM and PBM dry deposition simulation. Non-precipitation Hg wet deposition could play a crucial role in alpine and coastal regions, and its high uncertainties in both observation and simulation affect the overall uncertainties of Hg wet deposition. The overall uncertainties in the observation and simulation of the total global Hg deposition were estimated to be ± (25–50) % and ± (45–70) %, respectively, with the largest contributions from dry deposition. According to the results from uncertainty analysis, future research needs were recommended, among which a global Hg dry deposition network, unified methods for GOM and PBM dry deposition measurements, quantitative methods for GOM speciation, campaigns for comprehensive forest Hg behavior, and more efforts in long-term Hg deposition monitoring in Asia are the top priorities.


2019 ◽  
Author(s):  
Syuichi Itahashi ◽  
Baozhu Ge ◽  
Keiichi Sato ◽  
Joshua S. Fu ◽  
Xuemei Wang ◽  
...  

Abstract. The Model Inter-Comparison Study for Asia (MICS-Asia) Phase III was conducted to promote understanding of regional air quality and climate change in Asia, which have received growing attention due to the huge amount of anthropogenic emissions worldwide. This study provides an overview of acid depositions. Specifically, dry and wet depositions of the following species were analyzed: S (sulfate aerosol, sulfur dioxide (SO2), and sulfuric acid (H2SO4)), N (nitrate aerosol, nitrogen monoxide (NO), nitrogen dioxide (NO2), and nitric acid (HNO3)), and A (ammonium aerosol and ammonia (NH3)). The wet deposition simulated by a total of nine models was analyzed and evaluated using ground observation data from the Acid Deposition Monitoring Network in East Asia (EANET). In this Phase III study, the number of observation sites was increased to 54 from 37 in the Phase II study, and Southeast Asian countries were newly added. Additionally, whereas the analysis period was limited to representative months of each season in MICS-Asia Phase II, this Phase III study analyzed the full year of 2010. The scope of this overview mainly focuses on the annual accumulated depositions. In general, models can capture the observed wet depositions over Asia but underestimate the wet deposition of S and A and show large differences in the wet deposition of N. Furthermore, the ratio of wet deposition to the total deposition (the sum of dry and wet deposition) was investigated in order to understand the role of important processes in the total deposition. The general dominance of wet deposition over Asia and attributions from dry deposition over land were consistently found in all models. Then, total deposition maps over 13 countries participating in EANET were produced, and the balance between deposition and anthropogenic emissions was calculated. Excesses of deposition, rather than of anthropogenic emissions, were found over Japan, North Asia, and Southeast Asia, indicating the possibility of long-range transport within and outside Asia, as well as other emission sources. To improve the ability of models to capture the observed wet deposition, two approaches were attempted, namely, ensemble and precipitation adjustment. The ensemble approach was effective at modulating the differences in performance among models, and the precipitation-adjusted approach demonstrated that the model performance for precipitation played a key role in better simulating wet deposition. Finally, the lessons learned from this Phase III study and future perspectives for Phase IV are summarized.


2020 ◽  
Vol 20 (5) ◽  
pp. 2667-2693 ◽  
Author(s):  
Syuichi Itahashi ◽  
Baozhu Ge ◽  
Keiichi Sato ◽  
Joshua S. Fu ◽  
Xuemei Wang ◽  
...  

Abstract. The Model Inter-Comparison Study for Asia (MICS-Asia) phase III was conducted to promote understanding of regional air quality and climate change in Asia, which have received growing attention due to the huge amount of anthropogenic emissions worldwide. This study provides an overview of acid deposition. Specifically, dry and wet deposition of the following species was analyzed: S (sulfate aerosol, sulfur dioxide (SO2), and sulfuric acid (H2SO4)), N (nitrate aerosol, nitrogen monoxide (NO), nitrogen dioxide (NO2), and nitric acid (HNO3)), and A (ammonium aerosol and ammonia (NH3)). The wet deposition simulated by a total of nine models was analyzed and evaluated using ground observation data from the Acid Deposition Monitoring Network in East Asia (EANET). In the phase III study, the number of observation sites was increased from 37 in the phase II study to 54, and southeast Asian countries were newly added. Additionally, whereas the analysis period was limited to representative months of each season in MICS-Asia phase II, the phase III study analyzed the full year of 2010. The scope of this overview mainly focuses on the annual accumulated deposition. In general, models can capture the observed wet deposition over Asia but underestimate the wet deposition of S and A, and show large differences in the wet deposition of N. Furthermore, the ratio of wet deposition to the total deposition (the sum of dry and wet deposition) was investigated in order to understand the role of important processes in the total deposition. The general dominance of wet deposition over Asia and attributions from dry deposition over land were consistently found in all models. Then, total deposition maps over 13 countries participating in EANET were produced, and the balance between deposition and anthropogenic emissions was calculated. Excesses of deposition, rather than of anthropogenic emissions, were found over Japan, northern Asia, and southeast Asia, indicating the possibility of long-range transport within and outside of Asia, as well as other emission sources. To improve the ability of models to capture the observed wet deposition, two approaches were attempted, namely, ensemble and precipitation adjustment. The ensemble approach was effective at modulating the differences in performance among models, and the precipitation-adjusted approach demonstrated that the model performance for precipitation played a key role in better simulating wet deposition. Finally, the lessons learned from the phase III study and future perspectives for phase IV are summarized.


2012 ◽  
Vol 12 (1) ◽  
pp. 753-785 ◽  
Author(s):  
Y. P. Pan ◽  
Y. S. Wang ◽  
G. Q. Tang ◽  
D. Wu

Abstract. Emissions of reactive nitrogen (N) species can affect surrounding ecosystems via atmospheric deposition. However, few long-term and multi-site measurements have focused on both the wet and the dry deposition of individual N species in large areas of Northern China. Thus, the magnitude of atmospheric deposition of various N species in Northern China remains uncertain. In this study, the wet and dry atmospheric deposition of different N species was investigated during a three-year observation campaign at ten selected sites in Northern China. The results indicate that N deposition levels in Northern China were high with a ten-site, three-year average of 60.6 kg N ha−1 yr−1. The deposition levels showed spatial and temporal variation in the range of 28.5–100.4 kg N ha−1 yr−1. Of the annual total deposition, 40% was deposited via precipitation, and the remaining 60% was comprised of dry-deposited forms. Compared with gaseous N species, particulate N species were not the major contributor of dry-deposited N; they contributed approximately 10% to the total flux. On an annual basis, oxidized species accounted for 21% of total N deposition, thereby implying that other forms of gaseous N, such as NH3, comprised a dominant portion of the total flux. The contribution of NO3− to N deposition was enhanced in certain urban and industrial areas. As expected, the total N deposition in Northern China was significantly larger than the values reported by national scale monitoring networks in Europe, North America and East Asia because of high rates of wet deposition and gaseous NH3 dry deposition. The results have three important implications. First, atmospheric N deposition in Northern China falls within the range of critical loads for temperate forests and grasslands, a threshold above which harmful ecological effects to specified parts of temperate ecosystems often occur. Second, the magnitude, patterns and forms of N deposition will help to inform simulated N addition experiments, which are used to evaluate ecological impacts on receiving ecosystems. Third, the field-based evidence in this unique deposition dataset validates emission inventories of reactive N species and will help policy-makers control atmospheric pollution. Taken together, these findings show that NH3 emissions should be abated to mitigate high N deposition and associated potential impacts on ecosystems in Northern China.


2021 ◽  
Author(s):  
Shuoqiu Wu ◽  
Xiaoyan Ma

<p>The melting of glaciers and snow on the Qinghai-Tibet Plateau, known as the Earth’s “Third Pole” and “World Water Tower”, is source of fresh water for hundreds of millions of people in South Asia, Southeast Asia, and East Asia, but it is now suffering from an unprecedented crisis. The black carbon deposited on the surface of the glacier will reduce the snow albedo and absorb more solar radiation, leading to accelerated melting of ice and snow.Previous studies have shown that black carbon from South Asia is one of the main sources of the Qinghai-Tibet Plateau, and the transportation of black carbon to the Qinghai-Tibet Plateau presents obviously seasonal differences.However, the transport of black carbon from South Asia to the Qinghai-Tibet Plateau in different seasons shows a completely opposite trend to wind field conditions.This study uses the WRF-Chem model to study the transmission mechanism of South Asian black carbon to the Tibetan Plateau in April (pre-monsoon), July (summer monsoon) and December (winter monsoon).MIX emission inventory and Peking University's global black carbon emission inventory (PKU-BC) were involved to analyze the seasonal distribution of black carbon concentration, dry and wet deposition in the Qinghai-Tibet Plateau and South Asia, and the distribution of BC concentration and wind field at different altitudes.Combined with the vertical distribution of BC concentration across the Himalayas, the transport mechanism of black carbon in South Asia to Qinghai-Tibet Plateau in different seasons is studied.In the selected three months, December had the highest surface black carbon concentration in South Asia and the Qinghai-Tibet Plateau, while July had the lowest black carbon concentration; Mainly because of the large amount of wet deposition of black carbon brought about by the heavy precipitation in South Asia in July;According to the vertical distribution of black carbon,black carbon can climb up the hillside and eventually reach the southern slope of the Qinghai-Tibet Plateau in April. In July, black carbon is mainly distributed below 3km. In December, black carbon can be uplifted to 4-5km, and finally transported into Qinghai-Tibet Plateau.</p>


2018 ◽  
Author(s):  
David M. Nelson ◽  
Urumu Tsunogai ◽  
Ding Dong ◽  
Takuya Ohyama ◽  
Daisuke D. Komatsu ◽  
...  

Abstract. Atmospheric nitrate deposition resulting from anthropogenic activities negatively affects human and environmental health. Identifying deposited nitrate that is produced locally vs. that originating from long-distance transport would help inform efforts to mitigate such impacts. However, distinguishing the relative transport distances of atmospheric nitrate in urban areas remains a major challenge since it may be produced locally and/or come from upwind regions. To address this uncertainty we assessed spatiotemporal variation in monthly weighted-average Δ17O and δ15N values of wet and dry nitrate deposition during one year at urban and rural sites along the western coast of the northern Japanese island of Hokkaido, downwind of the East Asian continent. Δ17O values of nitrate in wet deposition at the urban site mirrored those of wet and dry deposition at the rural site, ranging between ~ +22 and +30 ‰ with higher values during winter and lower values in summer, which suggests greater relative importance of oxidation of NO2 by O3 during winter and OH during summer. In contrast, Δ17O values of nitrate in dry deposition at the urban site were lower (+19–+25 ‰) and displayed less distinct seasonal variation. Furthermore, the difference between δ15N values of nitrate in wet and dry nitrate deposition was, on average, 3 ‰ greater at the urban than rural site, and Δ17O and δ15N values were correlated for both forms of deposition at both sites with the exception of dry deposition at the urban site. These results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments forms from relatively greater oxidation of NO by peroxy radicals and/or oxidation of NO2 by OH. Given greater concentrations of peroxy radicals and OH in cities, these results imply that dry nitrate deposition results from local NOx emissions more so than wet deposition, which is transported longer distances. These results illustrate the value of stable isotope data for distinguishing the transport distances and reaction pathways of atmospheric nitrate pollution.


2011 ◽  
Vol 17 (12) ◽  
pp. 3589-3607 ◽  
Author(s):  
Lucy J. Sheppard ◽  
Ian D. Leith ◽  
Toshie Mizunuma ◽  
John Neil Cape ◽  
Alan Crossley ◽  
...  

2014 ◽  
Vol 14 (5) ◽  
pp. 2233-2244 ◽  
Author(s):  
J. Zhu ◽  
T. Wang ◽  
R. Talbot ◽  
H. Mao ◽  
X. Yang ◽  
...  

Abstract. A comprehensive measurement study of mercury wet deposition and size-fractionated particulate mercury (HgP) concurrent with meteorological variables was conducted from June 2011 to February 2012 to evaluate the characteristics of mercury deposition and particulate mercury in urban Nanjing, China. The volume-weighted mean (VWM) concentration of mercury in rainwater was 52.9 ng L−1 with a range of 46.3–63.6 ng L−1. The wet deposition per unit area was averaged 56.5 μg m−2 over 9 months, which was lower than that in most Chinese cities, but much higher than annual deposition in urban North America and Japan. The wet deposition flux exhibited obvious seasonal variation strongly linked with the amount of precipitation. Wet deposition in summer contributed more than 80% to the total amount. A part of contribution to wet deposition of mercury from anthropogenic sources was evidenced by the association between wet deposition and sulfates, as well as nitrates in rainwater. The ions correlated most significantly with mercury were formate, calcium, and potassium, which suggested that natural sources including vegetation and resuspended soil should be considered as an important factor to affect the wet deposition of mercury in Nanjing. The average HgP concentration was 1.10 ± 0.57 ng m−3. A distinct seasonal distribution of HgP concentrations was found to be higher in winter as a result of an increase in the PM10 concentration. Overall, more than half of the HgP existed in the particle size range less than 2.1 μm. The highest concentration of HgP in coarse particles was observed in summer, while HgP in fine particles dominated in fall and winter. The size distribution of averaged mercury content in particulates was bimodal, with two peaks in the bins of < 0.7 μm and 4.7–5.8 μm. Dry deposition per unit area of HgP was estimated to be 47.2 μg m−2 using meteorological conditions and a size-resolved particle dry deposition model. This was 16.5% less than mercury wet deposition. Compared to HgP in fine particles, HgP in coarse particles contributed more to the total dry deposition due to higher deposition velocities. Negative correlation between precipitation and the HgP concentration reflected the effect of scavenging of HgP by precipitation.


2016 ◽  
Author(s):  
Karin Haglund ◽  
Björn Claremar ◽  
Anna Rutgersson

Abstract. The shipping sector contributes significantly to increasing emissions of air pollutants. In order to achieve sustainable shipping, primarily through new regulations and techniques, greater knowledge of dispersion and deposition of air pollutants is required. Regional model calculations of the dispersion and deposition of sulphur, nitrogen and particulate matter from the international maritime sector in the Baltic Sea and the North Sea have been made for the years 2009 to 2013. In some areas in the Baltic Sea region the contribution of sulphur dioxide, nitrogen oxide and nitrogen dioxide from international shipping represented up to 80 % of the total near surface concentration of the pollutants. Contributions from shipping of PM2,5 and PM10 were calculated to a maximum of 21 % and 13 % respectively. The contribution of wet deposition of sulphur from shipping was maximum 29 % of the total wet deposition, and for dry deposition the contribution from shipping was maximum 84 %. The highest percentage contribution of wet deposition of nitrogen from shipping reached 28 % and for dry deposition 47 %. The highest concentrations and deposition of the pollutants in the study were found near large ports and shipping lanes. High concentrations were also found over larger areas at sea and over land where many people are exposed. With enhanced regulations for sulphur content in maritime fuel, the cleaning of exhausts through scrubbers has become a possible economic solution. Wet scrubbers meet the air quality criteria but their consequences for the marine environment are largely unknown. The resulting potential of future acidification in the Baltic Sea, both from atmospheric deposition and from open-loop scrubber water along the shipping lanes, based on different assumptions about sulphur content in fuel and scrubber usage has been assessed. Shipping is expected to increase globally and in the Baltic Sea region, deposition of sulphur due to shipping will depend on traffic density, emission regulations and technology choices for the emission controls. To evaluate future changes scenarios are developed considering the amount of scrubber technology used. The increase in deposition for the different scenarios differs slightly for the basins in the Baltic Sea. The proportion of ocean acidifying sulphur from ships increases when taking scrubber water into account and the major reason to increasing acidifying nitrogen from ships are due to increasing ship traffic. This study also generates a database of scenarios for atmospheric deposition and scrubber exhaust from the period 2011 to 2050.


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