scholarly journals Spatio-Temporal Variation of Atmospheric Gaseous and Particulate Reactive Nitrogen over Northern India

2021 ◽  
Vol Special Issue (1) ◽  
pp. 53-67
Author(s):  
Manisha Mishra ◽  
Umesh C Kulshrestha

The present study reports spatio-temporal distribution pattern of major gaseous (NH3 and NO2) and particulate water soluble total nitrogen (pWSTN) in the ambient air to explore the seasonal variation, major interactions and dominating sources. Considering the major hotspot of atmospheric reactive nitrogen (N) emission, three sites in Indo-Gangetic plain (IGP) were selected based on different local source parameters. Results have shown that gas phase reactive N contribute up to 90% of total analyzed reactive N, where NH3 imparted highest at all the three sites. Prayagraj, a fast growing urban site, has shown highest concentrations of NH3 (72.0 μg m−3), followed by Madhupur rural site (57.7 μg m−3) and Delhi, an urban megacity site (35.8 μg m−3). As compared to previous studies conducted at different sites of IGP, NH3 concentrations were reported to be the highest at the former two sites. However, unlike NH3, NO2 levels were recorded lower at Madhupur (3.1 μg m−3) and Prayagraj (9.4 μg m−3) sites as compared to Delhi (13.4 μg m−3). Similarly, pWSTN concentrations were in the order of Madhupur (6.6 μg m−3) < Prayagraj (10.0 μg m−3) < Delhi (10.1 μg m−3). A strong correlation of NO2 with pWSTN at urban sites has shown the crucial role of NO2 in the formation of nitrogenous aerosols. Significant spatial variation can be attributed to varying local emission sources ranging from microbial emission from improper sewage treatment and open waste dumping at Prayagraj, agricultural activities at Madhupur and vehicular exhausts at Delhi site.

2009 ◽  
Vol 9 (5) ◽  
pp. 1521-1535 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
N. Perron ◽  
L. Wacker ◽  
H.-A. Synal ◽  
...  

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Total carbon (TC) concentrations were 2.1–3.6 μg m−3, 1.8–1.9 μg m−3, and 2.2–3.0 μg m−3 for urban/winter, rural/winter, and urban/summer conditions, respectively. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood-burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were elevated only moderately at the rural compared to the urban site. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter.


2008 ◽  
Vol 8 (4) ◽  
pp. 16255-16289 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
L. Wacker ◽  
H.-A. Synal ◽  
M. Hallquist ◽  
...  

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were comparable at both sites. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter. The comparison of summer and winter results provides insight into the annual cycle of anthropogenic vs. biogenic contributions to the atmospheric aerosol.


2009 ◽  
Vol 9 (6) ◽  
pp. 23955-23986 ◽  
Author(s):  
S. Guo ◽  
M. Hu ◽  
Z. B. Wang ◽  
J. Slanina ◽  
Y. L. Zhao

Abstract. To characterize aerosol pollution in Beijing, size-resolved aerosols were collected by MOUDIs during CAREBEIJING-2006 field campaign at Peking University (urban site) and Yufa (upwind rural site). Fine particle concentrations (PM1.8 by MOUDI) were 99.8±77.4 μg/m3 and 78.2±58.4 μg/m3, with PM1.8/PM10 ratios of 0.64±0.08 and 0.76±0.08 at PKU and Yufa, respectively, and secondary compounds accounted for more than 50% in fine particles. PMF model was used to resolve the particle modes. Three modes were resolved at Yufa, representing condensation, droplet and coarse mode. However, one more droplet mode with bigger size was resolved, which was considered probably from regional transport. Condensation mode accounted for 10%–60% of the total mass at both sites, indicating it must be taken into account in summer. The formation of sulfate was mainly attributed to in-cloud or aerosol droplet process (PKU 80%, Yufa 70%) and gas condensation process (PKU 14%, Yufa 22%). According to the thermodynamic instability of NH4NO3, size distributions of nitrate were classified as three categories by RH. The existence of Ca(NO3)2 in droplet mode indicated the reaction of HNO3 with crustal particles was also important in fine particles. Linear regression gave a rough estimation that 69% of the PM10 and 87% of the PM1.8 at PKU were regional contributions. Sulfate, ammonium and oxalate were formed regionally, with the regional contributions of 90%, 87% and 95% to PM1.8. Nitrate formation was local dominant. In summary regional secondary formation led to aerosol pollution in the summer of Beijing.


2008 ◽  
Vol 8 (3) ◽  
pp. 10481-10530 ◽  
Author(s):  
W. Hua ◽  
Z. M. Chen ◽  
C. Y. Jie ◽  
Y. Kondo ◽  
A. Hofzumahaus ◽  
...  

Abstract. Atmospheric hydrogen peroxide (H2O2) and organic hydroperoxides were measured from 18 to 30 July in 2006 during the PRIDE-PRD'06 campaign at Backgarden, a rural site located 48 km north of Guangzhou, a mega-city in southern China. A ground-based instrument was used as a scrubbing coil collector to sample ambient air, followed by on-site analysis by high-performance liquid chromatography (HPLC) coupled with post-column derivatization and fluorescence detection. The H2O2 mixing ratio over the 13 days ranged from below the detection limit to a maximum of 4.6 ppbv, with a mean (and standard deviation) of (1.26±1.24) ppbv during the daytime (08:00–20:00 LT). Methyl hydroperoxide (MHP), with a maximum of 0.8 ppbv and a mean (and standard deviation) of (0.28±0.10) ppbv during the daytime, was the dominant organic hydroperoxide. Other organic peroxides, including bis-hydroxymethyl hydroperoxide (BHMP), peroxyacetic acid (PAA), hydroxymethyl hydroperoxide (HMHP), 1-hydroxy-ethyl hydroperoxide (1-HEHP) and ethyl hydroperoxide (EHP), were detected occasionally. The concentration of H2O2 exhibited a pronounced diurnal variation on sunny days, with a peak mixing ratio in the afternoon (12:00–18:00 LT), but lacked an explicit diurnal cycle on cloudy days. Sometimes a second peak mixing ratio of H2O2 was observed during the evening, suggesting that H2O2 was produced by the ozonolysis of alkenes. The diurnal variation profile of MHP was, in general, consistent with that of H2O2. The estimation indicated that in the morning the H2O2 detected was formed mostly through local photochemical activity, with the rest probably attributable to vertical transport. It is notable that relatively high levels of H2O2 and MHP were found in polluted air. The unexpectedly high level of HO2 radicals detected in this region can account for the production of hydroperoxides, while the high level of NOx suppressed the formation of hydroperoxides significantly. High concentrations of hydroperoxides were detected in samples of rainwater collected in a heavy shower on 25 July when a typhoon passed through, indicating that a considerable mixing ratio of hydroperoxides, particularly MHP, resided above the upper boundary layer, which might be transported on a regional scale and further influence the redistribution of HOx and ROx radicals. It was found that hydroperoxides, in particular H2O2, play an important role in the formation of secondary sulfate in the aerosol phase, where the heterogeneous reaction might contribute substantially. A negative correlation between hydroperoxides and water-soluble organic compounds (WSOC), a considerable fraction of the secondary organic aerosol (SOA), was observed, providing field evidence for the importance of hydroperoxides in the formation of SOA found in previous laboratory studies. We suggest that hydroperoxides act as an important link between sulfate and organic aerosols, which needs further study and should be considered in current atmospheric models.


2021 ◽  
Author(s):  
Manisha Mishra ◽  
Umesh Chandra Kulshrestha

Abstract Very limited information on the magnitude and environmental impacts of both inorganic as well as organic forms of Nitrogen (N) wet deposition is available in India. Molar concentrations of inorganic (NH4+ and NO3−) and organic N in rainwater were monitored at three different land-use sites in Indo-Gangetic Plain (IGP) during the monsoon period (June-September) of 2017. It has been observed that dissolved organic N (DON) contributed significantly to the total dissolved N (TDN) ranging from 5–60%. Dissolved inorganic N (DIN = NH4+ + NO3−) concentration was recorded as high as 221.0 µmol L− 1 at urban site to as low as 65.9 µmol L− 1 at the rural site. A similar pattern was also observed for DON. NH4+ contribution to TDN had the order: urban megacity (65%) > urban (70%) > rural (75%). Agriculture and animal husbandry are the primary sources of NH4+ emissions in the rural site. However, NO3− has shown a contrasting trend at these sites (25%, 15% and 8%, respectively). Wet deposition fluxes of atmospheric TDN was observed to be higher at urban sites. This can attributed to a variety of local sources such as vehicular emission, microbial emissions, biomass burning, human excreta due to higher population density, and transportation from surrounding areas, as observed from concentration weighted trajectories (CWT) model and cluster analysis. Upwind region of IGP has experienced major influence of air mass transported from agriculturally rich northwest part of India. However, both the downwind sites have experienced by-and-large the influence of south-westerly air-masses originated over the Arabian Sea. Study has found that the DON contributes significantly to TDN and need to be included for budget assessment in South Asia.


2008 ◽  
Vol 8 (22) ◽  
pp. 6755-6773 ◽  
Author(s):  
W. Hua ◽  
Z. M. Chen ◽  
C. Y. Jie ◽  
Y. Kondo ◽  
A. Hofzumahaus ◽  
...  

Abstract. Atmospheric hydrogen peroxide (H2O2) and organic hydroperoxides were measured from 18 to 30 July in 2006 during the PRIDE-PRD'06 campaign at Backgarden, a rural site located 48 km north of Guangzhou, a mega-city in southern China. A ground-based instrument was used as a scrubbing coil collector to sample ambient air, followed by on-site analysis by high-performance liquid chromatography (HPLC) coupled with post-column derivatization and fluorescence detection. The H2O2 mixing ratio over the 13 days ranged from below the detection limit to a maximum of 4.6 ppbv, with a mean (and standard deviation) of (1.26±1.24) ppbv during the daytime (08:00–20:00 LT). Methyl hydroperoxide (MHP), with a maximum of 0.8 ppbv and a mean (and standard deviation) of (0.28±0.10) ppbv during the daytime, was the dominant organic hydroperoxide. Other organic peroxides, including bis-hydroxymethyl hydroperoxide (BHMP), peroxyacetic acid (PAA), hydroxymethyl hydroperoxide (HMHP), 1-hydroxy-ethyl hydroperoxide (1-HEHP) and ethyl hydroperoxide (EHP), were detected occasionally. The concentration of H2O2 exhibited a pronounced diurnal variation on sunny days, with a peak mixing ratio in the afternoon (12:00–18:00 LT), but lacked an explicit diurnal cycle on cloudy days. Sometimes a second peak mixing ratio of H2O2 was observed during the evening, suggesting that H2O2 was produced by the ozonolysis of alkenes. The diurnal variation profile of MHP was, in general, consistent with that of H2O2. The estimation indicated that in the morning the H2O2 detected was formed mostly through local photochemical activity, with the rest probably attributable to vertical transport. It is notable that relatively high levels of H2O2 and MHP were found in polluted air. The unexpectedly high level of HO2 radicals detected in this region can account for the production of hydroperoxides, while the moderate level of NOx suppressed the formation of hydroperoxides. High concentrations of hydroperoxides were detected in samples of rainwater collected in a heavy shower on 25 July when a typhoon passed through, indicating that a considerable mixing ratio of hydroperoxides, particularly MHP, resided above the boundary layer, which might be transported on a regional scale and further influence the redistribution of HOx and ROx radicals. It was found that hydroperoxides, in particular H2O2, play an important role in the formation of secondary sulfate in the aerosol phase, where the heterogeneous reaction might contribute substantially. A negative correlation between hydroperoxides and water-soluble organic compounds (WSOC), a considerable fraction of the secondary organic aerosol (SOA), was observed, possibly providing field evidence for the importance of hydroperoxides in the formation of SOA found in previous laboratory studies. We suggest that hydroperoxides act as an important link between sulfate and organic aerosols, which needs further study and should be considered in current atmospheric models.


2012 ◽  
Vol 30 (10) ◽  
pp. 1479-1493 ◽  
Author(s):  
P. Choudhry ◽  
A. Misra ◽  
S. N. Tripathi

Abstract. Moderate resolution imaging spectroradiometer (MODIS) sensors, onboard Terra and Aqua, have been observing the Earth since start of 2000 and mid 2002, respectively. The present study provides a comparison of Collection 5 (C005), aerosol optical depth (AOD) retrieved by MODIS, with AERONET-observed AOD over Kanpur (an urban site), Gandhi College (a rural site) and Nainital (a relatively clean site) in the Indo Gangetic Plain (IGP). The results show that at Kanpur, MODIS retrievals are well within the prelaunch uncertainty ± 0.05 ±0.15 τ, and a good correlation (R2 > 0.7 for both Terra and Aqua). Nainital also shows good retrieval (R2 > 0.8 for Terra and R2 > 0.68 for Aqua), as more than 66% of total collocations are within the prelaunch uncertainty. However, it is seen that there is significant overestimation in this case, especially in the months of winter. Gandhi College poses a challenge to MODIS retrieval, as here <57% of MODIS-retrieved AOD values lay within the prelaunch uncertainty and the correlation is very poor (R2 ~ 0.5 for Aqua and R2 ~ 0.4 for Terra); also there is persistent underestimation in this case. Small value of slope shows that assumed model results in underestimation, and large intercept values for the linear regression fit show that errors due to surface reflectance are high here. Our comparison shows that MODIS retrieval works well over Kanpur, and Nainital with winter as an exception. However, MODIS retrieval is poor for Gandhi College which is a rural area. The aerosol properties at Kanpur are currently used as representative of the entire subcontinent in the MODIS C005 algorithm, which is not an accurate assumption. The large variability in land use and climate over India makes it a site too complex for a single aerosol model to be used over the entire area. Therefore further study with as many sites as possible over the Indian subcontinent would help provide more realistic modeling for the Indian subcontinent.


2010 ◽  
Vol 10 (3) ◽  
pp. 947-959 ◽  
Author(s):  
S. Guo ◽  
M. Hu ◽  
Z. B. Wang ◽  
J. Slanina ◽  
Y. L. Zhao

Abstract. To characterize aerosol pollution in Beijing, size-resolved aerosols were collected by MOUDIs during CAREBEIJING-2006 field campaign at Peking University (urban site) and Yufa (upwind rural site). Fine particle concentrations (PM1.8 by MOUDI) were 99.8±77.4 μg/m3 and 78.2±58.4 μg/m3, with PM1.8/PM10 ratios of 0.64±0.08 and 0.76±0.08 at PKU and Yufa, respectively, and secondary compounds accounted for more than 50% in fine particles. PMF model analysis was used to resolve the particle modes. Three modes were resolved at Yufa, representing condensation, droplet and coarse mode. However, one more droplet mode with bigger size was resolved, which was considered probably from regional transport. Condensation mode accounted for 10%–60% of the total mass at both sites, indicating that the gas-to-particle condensation process was important in summer. The formation of sulfate was mainly attributed to in-cloud or aerosol droplet process (PKU 80%, Yufa 70%) and gas condensation process (PKU 14%, Yufa 22%). According to the thermodynamic instability of NH4NO3, size distributions of nitrate were classified as three categories by RH. The existence of Ca(NO3)2 in droplet mode indicated the reaction of HNO3 with crustal particles was also important in fine particles. A rough estimation was given that 69% of the PM10 and 87% of the PM1.8 in Beijing urban were regional contributions. Sulfate, ammonium and oxalate were formed regionally, with the regional contributions of 90%, 87% and 95% to PM1.8. Nitrate formation was local dominant. In summary regional secondary formation led to aerosol pollution in the summer of Beijing.


2016 ◽  
Author(s):  
S. Sandrini ◽  
D. van Pinxteren ◽  
L. Giulianelli ◽  
H. Herrmann ◽  
L. Poulain ◽  
...  

Abstract. The aerosol size-segregated chemical composition was analyzed at an urban (Bologna) and a rural site (San Pietro Capofiume) in the Po Valley, Italy, during June and July 2012, to investigate sources and mechanisms of secondary aerosol formation during the summer. A significant enhancement of secondary organic and inorganic aerosol mass was observed under anticyclonic conditions with recirculation of planetary boundary layer air, but with substantial differences between the urban and the rural site. The data analysis, including a Principal Component Analysis (PCA) on the size-resolved dataset of chemical concentrations, indicated that the photochemical oxidation of inorganic and organic gaseous precursors was an important mechanism of secondary aerosol formation at both sites. In addition at the rural site a second formation process, explaining the largest fraction (22 %) of the total variance, was active at night-time, especially under stagnant conditions. Nocturnal chemistry in the rural Po Valley was associated with the formation of ammonium nitrate in large accumulation mode (0.42–1.2 µm) aerosols favored by local thermodynamic conditions (higher relative humidity and lower temperature compared to the urban site). Nocturnal concentrations of fine nitrate were, in fact, on average five times higher at the rural site than in Bologna. The water uptake by this highly hygroscopic compound under high RH conditions provided the medium for increased nocturnal aerosol uptake of water soluble organic gases and possibly also for aqueous chemistry, as revealed by the shifting of peak concentrations of secondary compounds (WSOC and sulfate) toward the large accumulation mode (0.42–1.2 µm). Contrarily, the diurnal production of WSOC (proxy for secondary organic aerosol) by photochemistry was similar at the two sites but mostly affected the small accumulation mode of particles (0.14–0.42 µm) in Bologna, while a shift to larger accumulation mode was observed at the rural site. A significant increment in carbonaceous aerosol concentration (for both WSOC and WINC) at the urban site was recorded mainly in the size range 0.05–0.14 µm indicating a direct influence of traffic emissions on the mass concentrations of quasi-ultrafine particles.


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