scholarly journals Estimation of NO<sub>x</sub> emissions from Delhi using Car MAX-DOAS observations and comparison with OMI satellite data

2011 ◽  
Vol 11 (21) ◽  
pp. 10871-10887 ◽  
Author(s):  
R. Shaiganfar ◽  
S. Beirle ◽  
M. Sharma ◽  
A. Chauhan ◽  
R. P. Singh ◽  
...  

Abstract. We present the first Multi-Axis-(MAX-) DOAS observations in India performed during April 2010 and January 2011 in Delhi and nearby regions. The MAX-DOAS instrument was mounted on a car roof, which allowed us to perform measurements along individual driving routes. From car MAX-DOAS observations along closed circles around Delhi, together with information on wind speed and direction, the NOx emissions from the greater Delhi area were determined: our estimate of 4.4 × 1025 molecules s−1 is found to be slightly lower than the corresponding emission estimates using the EDGAR emission inventory and substantially smaller compared to a recent study by Gurjar et al. (2004). We also determined NOx emissions from Delhi using OMI satellite observations on the same days. These emissions are slightly smaller than those from the car MAX-DOAS measurements. Finally the car MAX-DOAS observations were also used for the validation of simultaneous OMI satellite measurements of the tropospheric NO2 VCD and found a good agreement of the spatial patterns. Concerning the absolute values, OMI data are, on average, higher than the car MAX-DOAS observations close to strong emission sources, and vice versa over less polluted regions. Our results indicate that OMI NO2 VCDs are biased low over strongly polluted regions, probably caused by inadequate a-priori profiles used in the OMI satellite retrieval.

2011 ◽  
Vol 11 (7) ◽  
pp. 19179-19212 ◽  
Author(s):  
R. Shaiganfar ◽  
S. Beirle ◽  
M. Sharma ◽  
A. Chauhan ◽  
R. P. Singh ◽  
...  

Abstract. We present the first Multi-Axis- (MAX-) DOAS observations in India performed during April 2010 and January 2011 in Delhi and nearby regions. The MAX-DOAS instrument was mounted on a car roof, which allowed us to perform measurements along individual driving routes. From car MAX-DOAS observations along closed circles around Delhi, together with information on wind speed and direction, the NOx emissions from the greater Delhi area were determined: our estimate of 3.7 × 1025 molec s−1 is found to be slightly lower than the corresponding emission estimates using the EDGAR data base and substantially smaller compared to a recent study by Gurjar et al. (2004). We have also used the MAX-DOAS observations of the tropospheric NO2 VCD for validation of simultaneous satellite observations from the OMI instrument and found a good agreement of the spatial patterns. The absolute values show a reasonably good agreement. However, OMI data tends to underestimate the tropospheric NO2 VCDs in regions with high pollution levels, and tends to overestimate the tropospheric NO2 VCDs in more clean areas. These findings indicate possible discrepancies between the true vertical NO2 profiles and the profile assumptions in the OMI satellite retrieval.


2014 ◽  
Vol 14 (18) ◽  
pp. 10363-10381 ◽  
Author(s):  
G. C. M. Vinken ◽  
K. F. Boersma ◽  
J. D. Maasakkers ◽  
M. Adon ◽  
R. V. Martin

Abstract. Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 15 Tg N yr−1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). We use a state-of-science soil NOx emission inventory (Hudman et al., 2012) as a priori in the GEOS-Chem chemistry transport model to identify 11 regions where tropospheric NO2 columns are dominated by soil NOx emissions. Strong correlations between soil NOx emissions and simulated NO2 columns indicate that spatial patterns in simulated NO2 columns in these regions indeed reflect the underlying soil NOx emissions. Subsequently, we use a mass-balance approach to constrain emissions for these 11 regions on all major continents using OMI observed and GEOS-Chem simulated tropospheric NO2 columns. We find that responses of simulated NO2 columns to changing NOx emissions are suppressed over low NOx regions, and account for these non-linearities in our inversion approach. In general, our approach suggests that emissions need to be increased in most regions. Our OMI top-down soil NOx inventory amounts to 10.0 Tg N for 2005 when only constraining the 11 regions, and 12.9 Tg N when extrapolating the constraints globally. Substantial regional differences exist (ranging from −40% to +90%), and globally our top-down inventory is 4–35% higher than the GEOS-Chem a priori (9.6 Tg N yr−1). We evaluate NO2 concentrations simulated with our new OMI top-down inventory against surface NO2 measurements from monitoring stations in Africa, the USA and Europe. Although this comparison is complicated by several factors, we find an encouraging improved agreement when using the OMI top-down inventory compared to using the a priori inventory. To our knowledge, this study provides, for the first time, specific constraints on soil NOx emissions on all major continents using OMI NO2 columns. Our results rule out the low end of reported soil NOx emission estimates, and suggest that global emissions are most likely around 12.9 ± 3.9 Tg N yr−1.


2014 ◽  
Vol 14 (10) ◽  
pp. 14683-14724
Author(s):  
G. C. M. Vinken ◽  
K. F. Boersma ◽  
J. D. Maasakkers ◽  
M. Adon ◽  
R. V. Martin

Abstract. Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 27 Tg N yr−1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). We used a state-of-science soil NOx emission inventory (Hudman et al., 2012) as a priori in the GEOS-Chem chemistry transport model to identify 11 regions where tropospheric NO2 columns are dominated by soil NOx emissions. Strong correlations between soil NOx emissions and simulated NO2 columns indicated that spatial patterns in simulated NO2 columns in these regions indeed reflect the underlying soil NOx emissions. Subsequently, we used a mass-balance approach to constrain emissions for these 11 regions on all major continents using OMI observed and GEOS-Chem simulated tropospheric NO2 columns. We found that responses of simulated NO2 columns to changing NOx emissions were suppressed over low NOx regions, and accounted for these non-linearities in our inversion approach. In general, our approach suggests that emissions need to be increased in most regions. Our OMI top-down soil NOx inventory amounts to 10.0 Tg N for 2005 when only constraining the 11 regions, and 12.9 Tg N when extrapolating the constraints globally. Substantial regional differences exist (ranging from −40% to +90%), and globally our top-down inventory is 4–35% higher than the GEOS-Chem a priori (9.6 Tg N yr−1). We evaluated NO2 concentrations simulated with our new OMI top-down inventory against surface NO2 measurements from monitoring stations in Africa, the USA, and Europe. Although this comparison is complicated by several factors, we find an encouraging improved agreement when using the OMI top-down inventory compared to using the a priori inventory. To our knowledge, this study provides, for the first time, specific constraints on soil NOx emissions on all major continents using OMI NO2 columns. Our results rule out the high end of reported soil NOx emission estimates, and suggest that global emissions are most likely around 10–13 Tg N yr−1.


2016 ◽  
Author(s):  
Katherine R. Travis ◽  
Daniel J. Jacob ◽  
Jenny A. Fisher ◽  
Patrick S. Kim ◽  
Eloise A. Marais ◽  
...  

Abstract. Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NOx ≡ NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC4RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model (CTM) at 0.25°×0.3125° horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NOx from the US Environmental Protection Agency (EPA) is too high in the Southeast and nationally by 50 %. This is demonstrated by SEAC4RS observations of NOx and its oxidation products, by surface network observations of nitrate wet deposition fluxes, and by OMI satellite observations of tropospheric NO2 columns. Upper tropospheric NO2 from lightning makes a large contribution to the satellite observations that must be accounted for when using these data to estimate surface NOx emissions. Aircraft observations of upper tropospheric NO2 are higher than simulated by GEOS-Chem or expected from NO-NO2-O3 photochemical stationary state. NOx levels in the Southeast US are sufficiently low that only half of isoprene oxidation proceeds by the high-NOx pathway to produce ozone; this fraction is only moderately sensitive to changes in NOx emissions because isoprene and NOx emissions are spatially segregated. GEOS-Chem with reduced NOx emissions provides an unbiased simulation of ozone observations from the aircraft and from ozonesondes, and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NOx oxidation products. However, the model is still biased high by 8 ± 13 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to 0.2 km altitude, whereas GEOS-Chem has no such gradient because of efficient boundary layer mixing. We conclude that model biases in simulating surface ozone over the Southeast US may be due to a combination of excessive NOx emissions and excessive boundary layer vertical mixing.


2012 ◽  
Vol 12 (10) ◽  
pp. 4429-4447 ◽  
Author(s):  
S. W. Wang ◽  
Q. Zhang ◽  
D. G. Streets ◽  
K. B. He ◽  
R. V. Martin ◽  
...  

Abstract. Using OMI (Ozone Monitoring Instrument) tropospheric NO2 columns and a nested-grid 3-D global chemical transport model (GEOS-Chem), we investigated the growth in NOx emissions from coal-fired power plants and their contributions to the growth in NO2 columns in 2005–2007 in China. We first developed a unit-based power plant NOx emission inventory for 2005–2007 to support this investigation. The total capacities of coal-fired power generation have increased by 48.8% in 2005–2007, with 92.2% of the total capacity additions coming from generator units with size ≥300 MW. The annual NOx emissions from coal-fired power plants were estimated to be 8.11 Tg NO2 for 2005 and 9.58 Tg NO2 for 2007, respectively. The modeled summer average tropospheric NO2 columns were highly correlated (R2 = 0.79–0.82) with OMI measurements over grids dominated by power plant emissions, with only 7–14% low bias, lending support to the high accuracy of the unit-based power plant NOx emission inventory. The ratios of OMI-derived annual and summer average tropospheric NO2 columns between 2007 and 2005 indicated that most of the grids with significant NO2 increases were related to power plant construction activities. OMI had the capability to trace the changes of NOx emissions from individual large power plants in cases where there is less interference from other NOx sources. Scenario runs from GEOS-Chem model suggested that the new power plants contributed 18.5% and 10% to the annual average NO2 columns in 2007 in Inner Mongolia and North China, respectively. The massive new power plant NOx emissions significantly changed the local NO2 profiles, especially in less polluted areas. A sensitivity study found that changes of NO2 shape factors due to including new power plant emissions increased the summer average OMI tropospheric NO2 columns by 3.8–17.2% for six selected locations, indicating that the updated emission information could help to improve the satellite retrievals.


2011 ◽  
Vol 11 (12) ◽  
pp. 31523-31583 ◽  
Author(s):  
K. Miyazaki ◽  
H. J. Eskes ◽  
K. Sudo

Abstract. A data assimilation system has been developed to estimate global nitrogen oxides (NOx) emissions using OMI tropospheric NO2 columns (DOMINO product) and a global chemical transport model (CTM), CHASER. The data assimilation system, based on an ensemble Kalman filter approach, was applied to optimize daily NOx emissions with a horizontal resolution of 2.8° during the years 2005 and 2006. The background error covariance estimated from the ensemble CTM forecasts explicitly represents non-direct relationships between the emissions and tropospheric columns caused by atmospheric transport and chemical processes. In comparison to the a priori emissions based on bottom-up inventories, the optimized emissions were higher over Eastern China, the Eastern United States, Southern Africa, and Central-Western Europe, suggesting that the anthropogenic emissions are mostly underestimated in the inventories. In addition, the seasonality of the estimated emissions differed from that of the a priori emission over several biomass burning regions, with a large increase over Southeast Asia in April and over South America in October. The data assimilation results were validated against independent data: SCIAMACHY tropospheric NO2 columns and vertical NO2 profiles obtained from aircraft and lidar measurements. The emission correction greatly improved the agreement between the simulated and observed NO2 fields; this implies that the data assimilation system efficiently derives NOx emissions from concentration observations. We also demonstrated that biases in the satellite retrieval and model settings used in the data assimilation largely affect the magnitude of estimated emissions. These dependences should be carefully considered for better understanding NOx sources from top-down approaches.


2013 ◽  
Vol 13 (18) ◽  
pp. 9415-9438 ◽  
Author(s):  
E. V. Berezin ◽  
I. B. Konovalov ◽  
P. Ciais ◽  
A. Richter ◽  
S. Tao ◽  
...  

Abstract. Multiannual satellite measurements of tropospheric NO2 columns are used for evaluation of CO2 emission changes in China in the period from 1996 to 2008. Indirect top-down annual estimates of CO2 emissions are derived from the satellite NO2 column measurements by means of a simple inverse modeling procedure involving simulations performed with the CHIMERE mesoscale chemistry–transport model and the CO2-to-NOx emission ratios from the Emission Database for Global Atmospheric Research (EDGAR) global anthropogenic emission inventory and Regional Emission Inventory in Asia (REAS). Exponential trends in the normalized time series of annual emissions are evaluated separately for the periods from 1996 to 2001 and from 2001 to 2008. The results indicate that the both periods manifest strong positive trends in the CO2 emissions, and that the trend in the second period was significantly larger than the trend in the first period. Specifically, the trends in the first and second periods are best estimated to be in the range from 3.7 to 8.3 and from 11.0 to 13.2% per year, respectively, taking into account statistical uncertainties and differences between the CO2-to-NOx emission ratios from the EDGAR and REAS inventories. Comparison of our indirect top-down estimates of the CO2 emission changes with the corresponding bottom-up estimates provided by the EDGAR (version 4.2) and Global Carbon Project (GCP) glomal emission inventories reveals that while acceleration of the CO2 emission growth in the considered period is a common feature of both kinds of estimates, nonlinearity in the CO2 emission changes may be strongly exaggerated in the global emission inventories. Specifically, the atmospheric NO2 observations do not confirm the existence of a sharp bend in the emission inventory data time series in the period from 2000 to 2002. A significant quantitative difference is revealed between the bottom-up and indirect top-down estimates of the CO2 emission trend in the period from 1996 to 2001 (specifically, the trend was not positive according to the global emission inventories, but is strongly positive in our estimates). These results confirm the findings of earlier studies that indicated probable large uncertainties in the energy production and other activity data for China from international energy statistics used as the input information in the global emission inventories. For the period from 2001 to 2008, some quantitative differences between the different kinds of estimates are found to be in the range of possible systematic uncertainties associated with our estimation method. In general, satellite measurements of tropospheric NO2 are shown to be a useful source of information on CO2 sources collocated with sources of nitrogen oxides; the corresponding potential of these measurements should be exploited further in future studies.


2013 ◽  
Vol 13 (7) ◽  
pp. 17519-17544 ◽  
Author(s):  
B. Mijling ◽  
R. J. van der A ◽  
Q. Zhang

Abstract. Due to changing economic activity, emissions of air pollutants in East Asia change rapidly in space and time. Monthly emission estimates of nitrogen oxides derived from satellite observations provide valuable insight in the evolution of anthropogenic activity on a regional scale. We present the first results of a new emission estimation algorithm, specifically designed to use daily satellite observations of column concentrations for fast updates of emissions of short-lived atmospheric constituents on a~mesoscopic scale (~ 0.25° × 0.25°). The algorithm is used to construct a monthly NOx emission time series for 2007–2011 from tropospheric NO2 observations of GOME-2 for East Chinese provinces and surrounding countries. The new emission estimates correspond well with the bottom-up inventory of EDGAR v4.2, but are smaller than the inventories of INTEX-B and MEIC. They reveal a strong positive trend during 2007–2011 for almost all Chinese provinces, related to the country's economic development. We find a 41% increment of NOx emissions in East China during this period, which shows the need to update emission inventories in this region on a regular basis. Negative emission trends are found in Japan and South Korea, which can be attributed to a combined effect of local environmental policy and global economic crises. Analysis of seasonal variation distinguishes between regions with dominant anthropogenic or biogenic emissions. For regions with a mixed anthropogenic and biogenic signature, the opposite seasonality can be used for an estimation of the separate emission contributions. Finally, the non-local concentration/emission relationships calculated by the algorithm are used to quantify the direct effect of regional NOx emissions on tropospheric NO2 concentrations outside the region. For regions such as North Korea and Beijing province, a substantial part of the tropospheric NO2 originates from emissions elsewhere.


2021 ◽  
Author(s):  
Steffen Beirle ◽  
Steffen Dörner ◽  
Vinod Kumar ◽  
Thomas Wagner

&lt;p&gt;Satellite observations provide unique information on the amount and spatial distribution of tropospheric NO2. Several studies use such datasets for deriving NOx emissions. However, due to nonlinearities in the NOx chemistry (i.e., the dependency of the OH concentration and thus the NO2 lifetime on the NO2 concentration), the observed column densities of NO2 are not directly proportional to the underlying NOx emissions. Consequently, a certain reduction in NOx emissions could result in disproportionate reduction of the corresponding NO2 columns, which could be stronger or weaker depending on the chemical state (O3, NOx and VOC levels) and conditions like temperature, humidity and acitinic flux. This effect complicates the quantification of NOx emissions from satellite measurements of NO2, and e.g. biases the emission reduction as derived from the reduction of NO2 column densities observed during recent lockdowns. &amp;#160;&lt;/p&gt;&lt;p&gt;Here we quantify the nonlinearity of the NOx system for different cities as well as power plants by investigating the effect of reduced NOx emissions on days of rest, i.e. Fridays/Sundays in Muslim/Christian culture, respectively. The reduction of NOx emissions is thereby quantified based on the continuity equation by calculating the divergence of the mean NO2 flux. This method has been proven to be sensitive for localized sources, where the uncertainties due to NO2 lifetime are small (Beirle et al., Sci. Adv., 2019). This reduction in emissions is then set in relation to the corresponding reduction of NO2 columns integrated around the source, which strongly depend on the NO2 lifetime.&lt;/p&gt;


2019 ◽  
Vol 19 (13) ◽  
pp. 8863-8878 ◽  
Author(s):  
Rachel F. Silvern ◽  
Daniel J. Jacob ◽  
Loretta J. Mickley ◽  
Melissa P. Sulprizio ◽  
Katherine R. Travis ◽  
...  

Abstract. The National Emission Inventory (NEI) of the US Environmental Protection Agency (EPA) reports a steady decrease in US NOx emissions over the 2005–2017 period at a rate of 0.1 Tg N a−1 (53 % decrease over the period), reflecting sustained efforts to improve air quality. Tropospheric NO2 columns observed by the satellite-based Ozone Monitoring Instrument (OMI) over the US show a steady decrease until 2009 but a flattening afterward, which has been attributed to a flattening of NOx emissions, contradicting the NEI. We show here that the steady 2005–2017 decrease in NOx emissions reported by the NEI is in fact largely consistent with observed network trends of surface NO2 and ozone concentrations. The OMI NO2 trend is instead similar to that observed for nitrate wet deposition fluxes, which is weaker than that for anthropogenic NOx emissions, due to a large and increasing relative contribution of non-anthropogenic background sources of NOx (mainly lightning and soils). This is confirmed by contrasting OMI NO2 trends in urban winter, where the background is low and OMI NO2 shows a 2005–2017 decrease consistent with the NEI, and rural summer, where the background is high and OMI NO2 shows no significant 2005–2017 trend. A GEOS-Chem model simulation driven by NEI emission trends for the 2005–2017 period reproduces these different trends, except for the post-2009 flattening of OMI NO2, which we attribute to a model underestimate of free tropospheric NO2. Better understanding is needed of the factors controlling free tropospheric NO2 in order to relate satellite observations of tropospheric NO2 columns to the underlying NOx emissions and their trends. Focusing on urban winter conditions in the satellite data minimizes the effect of this free tropospheric background.


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