Temporal variability of primary and secondary aerosols over northern India: Impact of biomass burning emissions

2016 ◽  
Vol 125 ◽  
pp. 396-403 ◽  
Author(s):  
N. Rastogi ◽  
A. Singh ◽  
M.M. Sarin ◽  
D. Singh
2021 ◽  
Vol 21 (21) ◽  
pp. 16427-16452
Author(s):  
Shohei Nomura ◽  
Manish Naja ◽  
M. Kawser Ahmed ◽  
Hitoshi Mukai ◽  
Yukio Terao ◽  
...  

Abstract. Emissions of greenhouse gases (GHGs) from the Indian subcontinent have increased during the last 20 years along with rapid economic growth; however, there remains a paucity of GHG measurements for policy-relevant research. In northern India and Bangladesh, agricultural activities are considered to play an important role in GHG concentrations in the atmosphere. We performed weekly air sampling at Nainital (NTL) in northern India and Comilla (CLA) in Bangladesh from 2006 and 2012, respectively. Air samples were analyzed for dry-air gas mole fractions of CO2, CH4, CO, H2, N2O, and SF6 and carbon and oxygen isotopic ratios of CO2 (δ13C-CO2 and δ18O-CO2). Regional characteristics of these components over the Indo-Gangetic Plain are discussed compared to data from other Indian sites and Mauna Loa, Hawaii (MLO), which is representative of marine background air. We found that the CO2 mole fraction at CLA had two seasonal minima in February–March and September, corresponding to crop cultivation activities that depend on regional climatic conditions. Although NTL had only one clear minimum in September, the carbon isotopic signature suggested that photosynthetic CO2 absorption by crops cultivated in each season contributes differently to lower CO2 mole fractions at both sites. The CH4 mole fraction of NTL and CLA in August–October showed high values (i.e., sometimes over 4000 ppb at CLA), mainly due to the influence of CH4 emissions from the paddy fields. High CH4 mole fractions sustained over months at CLA were a characteristic feature on the Indo-Gangetic Plain, which were affected by both the local emission and air mass transport. The CO mole fractions at NTL were also high and showed peaks in May and October, while CLA had much higher peaks in October–March due to the influence of human activities such as emissions from biomass burning and brick production. The N2O mole fractions at NTL and CLA increased in June–August and November–February, which coincided with the application of nitrogen fertilizer and the burning of biomass such as the harvest residues and dung for domestic cooking. Based on H2 seasonal variation at both sites, it appeared that the emissions in this region were related to biomass burning in addition to production from the reaction of OH and CH4. The SF6 mole fraction was similar to that at MLO, suggesting that there were few anthropogenic SF6 emission sources in the district. The variability of the CO2 growth rate at NTL was different from the variability in the CO2 growth rate at MLO, which is more closely linked to the El Niño–Southern Oscillation (ENSO). In addition, the growth rates of the CH4 and SF6 mole fractions at NTL showed an anticorrelation with those at MLO, indicating that the frequency of southerly air masses strongly influenced these mole fractions. These findings showed that rather large regional climatic conditions considerably controlled interannual variations in GHGs, δ13C-CO2, and δ18O-CO2 through changes in precipitation and air mass.


2012 ◽  
Vol 5 (1) ◽  
pp. 1-66 ◽  
Author(s):  
R. Kumar ◽  
M. Naja ◽  
G. G. Pfister ◽  
M. C. Barth ◽  
C. Wiedinmyer ◽  
...  

Abstract. This study presents annual simulations of tropospheric ozone and related species made for the first time using the WRF-Chem model over South Asia for the year 2008. The model simulated ozone, CO, and NOx are evaluated against ground-based, balloon-borne and satellite-borne (TES, OMI and MOPITT) observations. The comparison of model results with surface ozone observations from seven sites and CO and NOx observations from three sites, indicate the model's ability in reproducing seasonal variations of ozone and CO, but show some differences in NOx. The modeled vertical ozone distribution agrees well with the ozone soundings data from two Indian sites. The vertical distributions of TES ozone and MOPITT CO are generally well reproduced, but the model underestimates TES ozone, OMI tropospheric column NO2 and MOPITT total column CO retrievals during all the months except MOPITT retrievals during August–January. Largest differences between modeled and satellite retrieved quantities are found during spring when intense biomass burning activity occurs in this region. The evaluation results indicate large uncertainties in anthropogenic and biomass burning emission estimates, especially for NOx. The model results indicate clear regional differences in the seasonality of surface ozone over South Asia with estimated net ozone production during daytime (11:30–15:30 h) over inland regions of 0–5 ppbv h−1 during all seasons and of 0–2 ppbv h−1 over marine regions during outflow periods. The model results indicate that ozone production in this region is mostly NOx-limited. This study shows that WRF-Chem model captures many important features of the observations and gives confidence to using the model for understanding the spatio-temporal variability of ozone over South Asia. However, improvements of South Asian emission inventories and simulations at finer model resolution, especially over the complex Himalayan terrain in Northern India, are also essential for accurately simulating ozone in this region.


2014 ◽  
Vol 14 (8) ◽  
pp. 3929-3943 ◽  
Author(s):  
P. Castellanos ◽  
K. F. Boersma ◽  
G. R. van der Werf

Abstract. Biomass burning is an important contributor to global total emissions of NOx (NO+NO2). Generally bottom-up fire emissions models calculate NOx emissions by multiplying fuel consumption estimates with static biome-specific emission factors, defined in units of grams of NO per kilogram of dry matter consumed. Emission factors are a significant source of uncertainty in bottom-up fire emissions modeling because relatively few observations are available to characterize the large spatial and temporal variability of burning conditions. In this paper we use NO2 tropospheric column observations from the Ozone Monitoring Instrument (OMI) from the year 2005 over South America to calculate monthly NOx emission factors for four fire types: deforestation, savanna/grassland, woodland, and agricultural waste burning. In general, the spatial patterns in NOx emission factors calculated in this work are consistent with emission factors derived from in situ measurements from the region but are more variable than published biome-specific global average emission factors widely used in bottom-up fire emissions inventories such as the Global Fire Emissions Database (GFED). Satellite-based NOx emission factors also indicate substantial temporal variability in burning conditions. Overall, we found that deforestation fires have the lowest NOx emission factors, on average 30% lower than the emission factors used in GFED v3. Agricultural fire NOx emission factors were the highest, on average a factor of 1.8 higher than GFED v3 values. For savanna, woodland, and deforestation fires, early dry season NOx emission factors were a factor of ~1.5–2 higher than late dry season emission factors. A minimum in the NOx emission factor seasonal cycle for deforestation fires occurred in August, the time period of severe drought in South America in 2005, supporting the hypothesis that prolonged dry spells may lead to an increase in the contribution of smoldering combustion from large-diameter fuels, offsetting the higher combustion efficiency of dryer fine fuels. We evaluated the OMI-derived NOx emission factors with SCIAMACHY NO2 tropospheric column observations and found improved model performance in regions dominated by fire emissions.


2016 ◽  
Vol 16 (13) ◽  
pp. 8309-8329 ◽  
Author(s):  
Yele Sun ◽  
Wei Du ◽  
Pingqing Fu ◽  
Qingqing Wang ◽  
Jie Li ◽  
...  

Abstract. Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size distributions, oxidation states of OA and evolutionary processes of secondary aerosols.


2011 ◽  
Vol 11 (15) ◽  
pp. 8133-8155 ◽  
Author(s):  
M. L. McGuire ◽  
C.-H. Jeong ◽  
J. G. Slowik ◽  
R. Y.-W. Chang ◽  
J. C. Corbin ◽  
...  

Abstract. An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range of temporal variability, enabling the elucidation of the determinants of aerosol chemical composition, including source emissions, chemical processing, and transport, at the Canada-US border. This paper presents the first study to elucidate the coupled influences of these determinants on temporal variability in aerosol chemical composition using single particle-type-based receptor modelling.


2012 ◽  
Vol 5 (3) ◽  
pp. 619-648 ◽  
Author(s):  
R. Kumar ◽  
M. Naja ◽  
G. G. Pfister ◽  
M. C. Barth ◽  
C. Wiedinmyer ◽  
...  

Abstract. This study presents annual simulations of tropospheric ozone and related species made for the first time using the WRF-Chem model over South Asia for the year 2008. The model-simulated ozone, CO, and NOx are evaluated against ground-based, balloon-borne and satellite-borne (TES, OMI and MOPITT) observations. The comparison of model results with surface ozone observations from seven sites and CO and NOx observations from three sites indicate the model's ability in reproducing seasonal variations of ozone and CO, but show some differences in NOx. The modeled vertical ozone distribution agrees well with the ozone soundings data from two Indian sites. The vertical distributions of TES ozone and MOPITT CO are generally well reproduced, but the model underestimates TES ozone, OMI tropospheric column NO2 and MOPITT total column CO retrievals during all the months, except MOPITT retrievals during August–January and OMI retrievals during winter. Largest differences between modeled and satellite-retrieved quantities are found during spring when intense biomass burning activity occurs in this region. The evaluation results indicate large uncertainties in anthropogenic and biomass burning emission estimates, especially for NOx. The model results indicate clear regional differences in the seasonality of surface ozone over South Asia, with estimated net ozone production during daytime (1130–1530 h) over inland regions of 0–5 ppbv h−1 during all seasons and of 0–2 ppbv h−1 over marine regions during outflow periods. The model results indicate that ozone production in this region is mostly NOx-limited. This study shows that WRF-Chem model captures many important features of the observations and gives confidence to using the model for understanding the spatio-temporal variability of ozone over South Asia. However, improvements of South Asian emission inventories and simulations at finer model resolution, especially over the complex Himalayan terrain in northern India, are also essential for accurately simulating ozone in this region.


2013 ◽  
Vol 13 (8) ◽  
pp. 22757-22793 ◽  
Author(s):  
P. Castellanos ◽  
K. F. Boersma ◽  
G. R. van der Werf

Abstract. Biomass burning is an important contributor to global total emissions of NOx (NO + NO2). Generally bottom-up fire emissions models calculate NOx emissions by multiplying fuel consumption estimates with static biome specific emission factors, defined in units of grams of NO per kilogram of dry matter consumed. Emission factors are a significant source of uncertainty in bottom-up fire emissions modeling because relatively few observations are available to characterize the large spatial and temporal variability of burning conditions. In this paper we use NO2 tropospheric column observations from the Ozone Monitoring Instrument (OMI) from the year 2005 over South America to calculate monthly NOx emission factors for four fire types: deforestation, savanna/grassland, woodland, and agricultural waste burning. In general, the spatial trends in NOx emission factors calculated in this work are consistent with emission factors derived from in situ measurements from the region, but are more variable than published biome specific global average emission factors widely used in bottom up fire emissions inventories such as the Global Fire Emissions Database (GFED) v3. Satellite based NOx emission factors also indicate substantial temporal variability in burning conditions. Overall, we found that deforestation fires have the lowest NOx emission factors, on average 30 % lower than the emission factors used in GFED v3. Agricultural fire NOx emission factors were the highest, on average a factor of 2 higher than GFED v3 values. For savanna, woodland, and deforestation fires early dry season NOx emission factors were a factor of ~1.5–2.0 higher than late dry season emission factors. A minimum in the NOx emission factor seasonal cycle for deforestation fires occurred in August, the time period of severe drought in South America in 2005. Our results support the hypothesis that prolonged dry spells may lead to an increase in the contribution of smoldering combustion from large diameter fuels to total fire emissions, which would lower the overall modified combustion efficiency (MCE) and NOx emission factor, and offset the higher combustion efficiency of dryer fine fuels. We evaluated the OMI derived NOx emission factors with SCIAMACHY NO2 tropospheric column observations and found improved model performance in regions dominated by fire emissions.


Author(s):  
Nishit Aman ◽  
Kasemsan Manomaiphiboon ◽  
Natchanok Pala-En ◽  
Eakkachai Kokkaew ◽  
Tassana Boonyoo ◽  
...  

This present work investigates several local and synoptic meteorological aspects associated with two wintertime haze episodes in Greater Bangkok using observational data, covering synoptic patterns evolution, day-to-day and diurnal variation, dynamic stability, temperature inversion, and back-trajectories. The episodes include an elevated haze event of 16 days (14–29 January 2015) for the first episode and 8 days (19–26 December 2017) for the second episode, together with some days before and after the haze event. Daily PM2.5 was found to be 50 µg m−3 or higher over most of the days during both haze events. These haze events commonly have cold surges as the background synoptic feature to initiate or trigger haze evolution. A cold surge reached the study area before the start of each haze event, causing temperature and relative humidity to drop abruptly initially but then gradually increased as the cold surge weakened or dissipated. Wind speed was relatively high when the cold surge was active. Global radiation was generally modulated by cloud cover, which turns relatively high during each haze event because cold surge induces less cloud. Daytime dynamic stability was generally unstable along the course of each haze event, except being stable at the ending of the second haze event due to a tropical depression. In each haze event, low-level temperature inversion existed, with multiple layers seen in the beginning, effectively suppressing atmospheric dilution. Large-scale subsidence inversion aloft was also persistently present. In both episodes, PM2.5 showed stronger diurnality during the time of elevated haze, as compared to the pre- and post-haze periods. During the first episode, an apparent contrast of PM2.5 diurnality was seen between the first and second parts of the haze event with relatively low afternoon PM2.5 over its first part, but relatively high afternoon PM2.5 over its second part, possibly due to the role of secondary aerosols. PM2.5/PM10 ratio was relatively lower in the first episode because of more impact of biomass burning, which was in general agreement with back-trajectories and active fire hotspots. The second haze event, with little biomass burning in the region, was likely to be caused mainly by local anthropogenic emissions. These findings suggest a need for haze-related policymaking with an integrated approach that accounts for all important emission sectors for both particulate and gaseous precursors of secondary aerosols. Given that cold surges induce an abrupt change in local meteorology, the time window to apply control measures for haze is limited, emphasizing the need for readiness in mitigation responses and early public warning.


2016 ◽  
Author(s):  
Yele Sun ◽  
Wei Du ◽  
Pingqing Fu ◽  
Qingqing Wang ◽  
Jie Li ◽  
...  

Abstract. Winter has the worst air pollution in a year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge on the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from December 17, 2013 to January 17, 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was overall similar in winter among different years, which was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions, and two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56% with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g., CH2SO2+) was identified. aq-OOA on average contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size distributions, oxidation states of OA, and evolutionary processes of secondary aerosols.


Sign in / Sign up

Export Citation Format

Share Document