scholarly journals A top-down assessment using OMI NO2 suggests an underestimate in the NOx emissions inventory in Seoul, South Korea during KORUS-AQ

Author(s):  
Daniel L. Goldberg ◽  
Pablo E. Saide ◽  
Lok N. Lamsal ◽  
Benjamin de Foy ◽  
Zifeng Lu ◽  
...  

Abstract. In this work, we investigate the NOx emissions inventory in Seoul, South Korea using a regional NASA Ozone Monitoring Instrument (OMI) NO2 product. We first develop a regional OMI NO2 product by re-calculating the air mass factors using a high-resolution (4 × 4 km2) WRF-Chem model simulation, which better captures the NO2 shape profiles in urban regions. We then apply a model-derived spatial averaging kernel to further downscale the retrieval and account for the sub-pixel variability. These two modifications yield OMI NO2 values in the regional product that are 1.37 larger in the Seoul metropolitan region and > 2 times larger near large industrial sources. These two modifications also yield an OMI NO2 product that is in better agreement with the Pandora NO2 spectrometer measurements acquired during the Korea U.S.-Air Quality (KORUS-AQ) field campaign. NOx emissions are then derived for the Seoul metropolitan area during the KORUS-AQ field campaign using a top-down approach with the standard and regional NASA OMI NO2 products. We first apply the top-down approach to a model simulation to ensure that the method is appropriate: the WRF-Chem simulation utilizing the bottom-up emission inventory yields a NOx emission rate of 227 ± 94 kton/yr, while the bottom-up inventory itself yields a NOx emission rate of 198 kton/yr. Using the top-down approach on the regional OM NO2 product, we derive the NOx emissions rate from Seoul to be 484 ± 201 kton/yr, and a 353 ± 146 kton/yr NOx emissions rate using the standard NASA OMI NO2 product. This suggests an underestimate of 53 % and 36 % using the regional and standard NASA OMI NO2 products respectively. To supplement this finding, we compare the NO2 simulated by WRF-Chem to observations of the same quantity acquired by aircraft and find a model underestimate. When NOx emissions in the WRF-Chem model are doubled, there is better agreement with KORUS-AQ aircraft observations. Although the current work is focused on South Korea using OMI, the methodology developed in this work can be applied to other world regions using TROPOMI and future satellite datasets (e.g., GEMS and TEMPO) to produce high-quality region-specific top-down NOx emission estimates.

2019 ◽  
Vol 19 (3) ◽  
pp. 1801-1818 ◽  
Author(s):  
Daniel L. Goldberg ◽  
Pablo E. Saide ◽  
Lok N. Lamsal ◽  
Benjamin de Foy ◽  
Zifeng Lu ◽  
...  

Abstract. In this work, we investigate the NOx emissions inventory in Seoul, South Korea, using a regional ozone monitoring instrument (OMI) NO2 product derived from the standard NASA product. We first develop a regional OMI NO2 product by recalculating the air mass factors using a high-resolution (4 km × 4 km) WRF-Chem model simulation, which better captures the NO2 profile shapes in urban regions. We then apply a model-derived spatial averaging kernel to further downscale the retrieval and account for the subpixel variability. These two modifications yield OMI NO2 values in the regional product that are 1.37 times larger in the Seoul metropolitan region and >2 times larger near substantial point sources. These two modifications also yield an OMI NO2 product that is in better agreement with the Pandora NO2 spectrometer measurements acquired during the South Korea–United States Air Quality (KORUS-AQ) field campaign. NOx emissions are then derived for the Seoul metropolitan area during the KORUS-AQ field campaign using a top-down approach with the standard and regional NASA OMI NO2 products. We first apply the top-down approach to a model simulation to ensure that the method is appropriate: the WRF-Chem simulation utilizing the bottom-up emissions inventory yields a NOx emissions rate of 227±94 kt yr−1, while the bottom-up inventory itself within a 40 km radius of Seoul yields a NOx emissions rate of 198 kt yr−1. Using the top-down approach on the regional OMI NO2 product, we derive the NOx emissions rate from Seoul to be 484±201 kt yr−1, and a 353±146 kt yr−1 NOx emissions rate using the standard NASA OMI NO2 product. This suggests an underestimate of 53 % and 36 % in the bottom-up inventory using the regional and standard NASA OMI NO2 products respectively. To supplement this finding, we compare the NO2 and NOy simulated by WRF-Chem to observations of the same quantity acquired by aircraft and find a model underestimate. When NOx emissions in the WRF-Chem model are increased by a factor of 2.13 in the Seoul metropolitan area, there is better agreement with KORUS-AQ aircraft observations and the recalculated OMI NO2 tropospheric columns. Finally, we show that by using a WRF-Chem simulation with an updated emissions inventory to recalculate the air mass factor (AMF), there are small differences (∼8 %) in OMI NO2 compared to using the original WRF-Chem simulation to derive the AMF. This suggests that changes in model resolution have a larger effect on the AMF calculation than modifications to the South Korean emissions inventory. Although the current work is focused on South Korea using OMI, the methodology developed in this work can be applied to other world regions using TROPOMI and future satellite datasets (e.g., GEMS and TEMPO) to produce high-quality region-specific top-down NOx emissions estimates.


2021 ◽  
Author(s):  
Richard J. Pope ◽  
Rebecca Kelly ◽  
Eloise A. Marais ◽  
Ailish M. Graham ◽  
Chris Wilson ◽  
...  

Abstract. Nitrogen oxides (NOx, NO+NO2) are potent air pollutants which directly impact on human health and which aid the formation of other hazardous pollutants such as ozone (O3) and particulate matter. In this study, we use satellite tropospheric column nitrogen dioxide (TCNO2) data to evaluate the spatiotemporal variability and magnitude of the United Kingdom (UK) bottom-up National Atmospheric Emissions Inventory (NAEI) NOx emissions. Although emissions and TCNO2 represent different quantities, for UK city sources we find a spatial correlation of ~0.5 between the NAEI NOx emissions and TCNO2 from the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI), suggesting a good spatial distribution of emission sources in the inventory. Between 2005 and 2015, the NAEI total UK NOx emissions and long-term TCNO2 record from the Ozone Monitoring Instrument (OMI), averaged over England, show decreasing trends of 4.4 % and 2.2 %, respectively. Top-down NOx emissions were derived in this study by applying a simple mass balance approach to TROPOMI observed downwind NO2 plumes from city sources. Overall, these top-down estimates were consistent with the NAEI, but for larger cities such as London and Manchester the inventory is significantly (> 25 %) less than the top-down emissions. This NAEI NOx emission underestimate is supported by comparing simulations from the GEOS-Chem atmospheric chemistry model, driven by the NAEI emissions, with satellite and surface NO2 observations over the UK. This yields substantial model negative biases, providing further evidence to demonstrate that the NAEI may be underestimating NOx emissions in London and Manchester.


2020 ◽  
Author(s):  
Yang Yang ◽  
Yu Zhao ◽  
Lei Zhang ◽  
Jie Zhang ◽  
Xin Huang ◽  
...  

Abstract. We developed a top-down methodology combining the inversed chemistry transport modeling and satellite-derived tropospheric vertical column of NO2, and estimated the NOx emissions of Yangtze River Delta (YRD) region at a horizontal resolution of 9 km for January, April, July and October 2016. The effect of the top-down emission estimation on air quality modeling, and the response of ambient ozone (O3) and secondary inorganic aerosols (SO42−, NO3−, and NH4+, SNA) to the changed precursor emissions were evaluated with the Community Multi-scale Air Quality (CMAQ) system. The top-down estimates of NOx emissions were smaller than those in a national emission inventory, MEIC (i.e., the bottom-up estimates), for all the four months, and the monthly mean was calculated at 260.0 Gg/month, 24 % less than the bottom-up one. The NO2 concentrations simulated with the bottom-up estimate of NOx emissions were clearly higher than the ground observation, indicating the possible overestimation in current emission inventory attributed to its insufficient consideration of recent emission control in the region. The model performance based on top-down estimate was much better, and the biggest change was found for July with the normalized mean bias (NMB) and normalized mean error (NME) reduced from 111 % to −0.4 % and from 111 % to 33 %, respectively. The results demonstrate the improvement of NOx emission estimation with the nonlinear inversed modeling and satellite observation constraint. With the smaller NOx emissions in the top-down estimate than the bottom-up one, the elevated concentrations of ambient O3 were simulated for most YRD and they were closer to observation except for July, implying the VOC (volatile organic compound)-limit regime of O3 formation. With available ground observations of SNA in the YRD, moreover, better model performance of NO3− and NH4+ were achieved for most seasons, implying the effectiveness of precursor emission estimation on the simulation of secondary inorganic aerosols. Through the sensitivity analysis of O3 formation for April 2016, the decreased O3 concentrations were found for most YRD region when only VOCs emissions were reduced or the reduced rate of VOCs emissions was two times of that of NOx, implying the crucial role of VOCs control on O3 pollution abatement. The SNA level for January 2016 was simulated to decline 12 % when 30 % of NH3 emissions were reduced, while the change was much smaller with the same reduced rate for SO2 or NOx. The result suggests that reducing NH3 emissions was the most effective way to alleviate SNA pollution for YRD in winter.


2020 ◽  
Author(s):  
Rokjin Park ◽  
Hyeong-Ahn Kwon ◽  
Yujin Oak

<p>The Geostationary Environment Monitoring Spectrometer (GEMS) will be launched in February 2020 and will provide hourly observations of atmospheric compositions in the daytime. Prior to the GEMS launch, we explore an application of GEMS data as constraints for estimating anthropogenic volatile organic compound (AVOC) emissions in South Korea using formaldehyde (HCHO) vertical column densities observations from the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) onboard the B200 aircraft during the KORUS-AQ campaign. Our top-down estimates of total AVOC emissions are higher by a factor of four over the petrochemical industries compared to the bottom-up emissions. However, the national AVOC emissions from the top-down estimates are by 37% lower than those of the bottom-up emission inventory in South Korea. We also show that hourly column observations of HCHO can improve not only the total magnitude of AVOC emissions but also their diurnal variation, which is poorly constrained and used in air quality models. Our hourly estimates of AVOC emissions may, thus, improve air quality model simulations in which the simulated ozone sensitivity to AVOC emission changes are also investigated.</p>


2009 ◽  
Vol 9 (17) ◽  
pp. 6305-6317 ◽  
Author(s):  
M. Zavala ◽  
S. C. Herndon ◽  
E. C. Wood ◽  
T. B. Onasch ◽  
W. B. Knighton ◽  
...  

Abstract. Mobile emissions represent a significant fraction of the total anthropogenic emissions burden in the Mexico City Metropolitan Area (MCMA) and, therefore, it is crucial to use top-down techniques informed by on-road exhaust measurements to evaluate and improve traditional bottom-up official emissions inventory (EI) for the city. We present the measurements of on-road fleet-average emission factors obtained using the Aerodyne mobile laboratory in the MCMA in March 2006 as part of the MILAGRO/MCMA-2006 field campaign. A comparison of our on-road emission measurements with those obtained in 2003 using essentially the same measurement techniques and analysis methods indicates that, in the three year span, NO emission factors remain within the measured variability ranges whereas emission factors of aldehydes and aromatics species were reduced for all sampled driving conditions. We use a top-down fuel-based approach to evaluate the mobile emissions from the gasoline fleet estimated in the bottom-up official 2006 MCMA mobile sources. Within the range of measurement uncertainties, we found probable slight overpredictions of mean EI estimates on the order of 20–28% for CO and 14–20% for NO. However, we identify a probable EI discrepancy of VOC mobile emissions between 1.4 and 1.9; although estimated benzene and toluene mobile emissions in the inventory seem to be well within the uncertainties of the corresponding emissions estimates. Aldehydes mobile emissions in the inventory, however, seem to be underpredicted by factors of 3 for HCHO and 2 for CH3CHO. Our on-road measurement-based estimate of annual emissions of organic mass from PM1 particles suggests a severe underprediction (larger than a factor of 4) of PM2.5 mobile emissions in the inventory. Analyses of ambient CO, NOx and CO/NOx concentration trends in the MCMA indicate that the early morning ambient CO/NOx ratio has decreased at a rate of about 1.9 ppm/ppm/year over the last two decades due to reductions in CO levels rather than by NOx. These trends, together with the analysis of fuel sales and fleet size, suggest that the relative contribution of diesel vehicles to overall NOx levels has increased over time in the city. Despite the impressive increase in the size of the vehicle fleet between 2000 and 2006, the early morning ambient concentrations of CO and NOx have not increased accordingly, probably due to the reported low removal rates of older vehicles, which do not have emissions control technologies, and partially due to the much lower emissions from newer gasoline vehicles. This indicates that an emission-based air quality improvement strategy targeting large reductions of emissions from mobile sources should be directed towards a significant increase of the removal rate of older, highly-polluting, vehicles.


2018 ◽  
Vol 7 (2) ◽  
pp. 52-60
Author(s):  
Francis Olawale Abulude ◽  
Moez Bahloul ◽  
Smart Olubayode ◽  
Ebenezer Alaba Adeoya

AbstractIt is a well-known fa ct that pollution is a global problem and mus t be holis ticall y ta ckled. In doing this, a dequa te knowledge of the sources of pollution is i mporta nt; therefore, the ai m of this paper is to review source a pportionment wi th reference to top-down and bottom-up methods . In this paper, dispersion modelling, emissions inventory and sa mpling methods are dis cussed. Also, anal yti cal methods invol ved in top -down source apportionment a re mentioned. The two techniques are needed to evalua te pollutants and their sources . Based on these two approa ches , pollution control s tra tegy is developed and decisions can be made on deci ding the ri ght approach to sol ve or reduce the pollution problems .


2021 ◽  
Vol 21 (2) ◽  
pp. 1191-1209
Author(s):  
Yang Yang ◽  
Yu Zhao ◽  
Lei Zhang ◽  
Jie Zhang ◽  
Xin Huang ◽  
...  

Abstract. We developed a top-down methodology combining the inversed chemistry transport modeling and satellite-derived tropospheric vertical column of NO2 and estimated the NOx emissions of the Yangtze River Delta (YRD) region at a horizontal resolution of 9 km for January, April, July, and October 2016. The effect of the top-down emission estimation on air quality modeling and the response of ambient ozone (O3) and inorganic aerosols (SO42-, NO3-, and NH4+, SNA) to the changed precursor emissions were evaluated with the Community Multi-scale Air Quality (CMAQ) system. The top-down estimates of NOx emissions were smaller than those (i.e., the bottom-up estimates) in a national emission inventory, Multi-resolution Emission Inventory for China (MEIC), for all the 4 months, and the monthly mean was calculated to be 260.0 Gg/month, 24 % less than the bottom-up one. The NO2 concentrations simulated with the bottom-up estimate of NOx emissions were clearly higher than the ground observations, indicating the possible overestimation in the current emission inventory, attributed to its insufficient consideration of recent emission control in the region. The model performance based on top-down estimate was much better, and the biggest change was found for July, with the normalized mean bias (NMB) and normalized mean error (NME) reduced from 111 % to −0.4 % and from 111 % to 33 %, respectively. The results demonstrate the improvement of NOx emission estimation with the nonlinear inversed modeling and satellite observation constraint. With the smaller NOx emissions in the top-down estimate than the bottom-up one, the elevated concentrations of ambient O3 were simulated for most of the YRD, and they were closer to observations except for July, implying the VOC (volatile organic compound)-limited regime of O3 formation. With available ground observations of SNA in the YRD, moreover, better model performance of NO3- and NH4+ was achieved for most seasons, implying the effectiveness of precursor emission estimation on the simulation of secondary inorganic aerosols. Through the sensitivity analysis of O3 formation for April 2016, the decreased O3 concentrations were found for most of the YRD region when only VOC emissions were reduced or the reduced rate of VOC emissions was 2 times of that of NOx, implying the crucial role of VOC control in O3 pollution abatement. The SNA level for January 2016 was simulated to decline 12 % when 30 % of NH3 emissions were reduced, while the change was much smaller with the same reduced rate for SO2 or NOx. The result suggests that reducing NH3 emissions was the most effective way to alleviate SNA pollution of the YRD in winter.


2015 ◽  
Vol 15 (18) ◽  
pp. 10367-10383 ◽  
Author(s):  
Z. Lu ◽  
D. G. Streets ◽  
B. de Foy ◽  
L. N. Lamsal ◽  
B. N. Duncan ◽  
...  

Abstract. Satellite remote sensing of tropospheric nitrogen dioxide (NO2) can provide valuable information for estimating surface nitrogen oxides (NOx) emissions. Using an exponentially modified Gaussian (EMG) method and taking into account the effect of wind on observed NO2 distributions, we estimate 3-year moving-average emissions of summertime NOx from 35 US (United States) urban areas directly from NO2 retrievals of the Ozone Monitoring Instrument (OMI) during 2005–2014. Following conclusions of previous studies that the EMG method provides robust and accurate emission estimates under strong-wind conditions, we derive top-down NOx emissions from each urban area by applying the EMG method to OMI data with wind speeds greater than 3–5 m s−1. Meanwhile, we find that OMI NO2 observations under weak-wind conditions (i.e., < 3 m s−1) are qualitatively better correlated to the surface NOx source strength in comparison to all-wind OMI maps; therefore, we use them to calculate the satellite-observed NO2 burdens of urban areas and compare with NOx emission estimates. The EMG results show that OMI-derived NOx emissions are highly correlated (R > 0.93) with weak-wind OMI NO2 burdens as well as with bottom-up NOx emission estimates over 35 urban areas, implying a linear response of the OMI observations to surface emissions under weak-wind conditions. The simultaneous EMG-obtained effective NO2 lifetimes (~ 3.5 ± 1.3 h), however, are biased low in comparison to the summertime NO2 chemical lifetimes. In general, isolated urban areas with NOx emission intensities greater than ~ 2 Mg h−1 produce statistically significant weak-wind signals in 3-year average OMI data. From 2005 to 2014, we estimate that total OMI-derived NOx emissions over all selected US urban areas decreased by 49 %, consistent with reductions of 43, 47, 49, and 44 % in the total bottom-up NOx emissions, the sum of weak-wind OMI NO2 columns, the total weak-wind OMI NO2 burdens, and the averaged NO2 concentrations, respectively, reflecting the success of NOx control programs for both mobile sources and power plants. The decrease rates of these NOx-related quantities are found to be faster (i.e., −6.8 to −9.3 % yr−1) before 2010 and slower (i.e., −3.4 to −4.9 % yr−1) after 2010. For individual urban areas, we calculate the R values of pair-wise trends among the OMI-derived and bottom-up NOx emissions, the weak-wind OMI NO2 burdens, and ground-based NO2 measurements, and high correlations are found for all urban areas (median R= 0.8), particularly large ones (R up to 0.97). The results of the current work indicate that using the EMG method and considering the wind effect, the OMI data allow for the estimation of NOx emissions from urban areas and the direct constraint of emission trends with reasonable accuracy.


2009 ◽  
Vol 9 (3) ◽  
pp. 1017-1036 ◽  
Author(s):  
K. M. Han ◽  
C. H. Song ◽  
H. J. Ahn ◽  
R. S. Park ◽  
J. H. Woo ◽  
...  

Abstract. In this study, NO2 columns from the US EPA Models-3/CMAQ model simulations carried out using the 2001 ACE-ASIA (Asia Pacific Regional Aerosol Characterization Experiment) emission inventory over East Asia were compared with the GOME-derived NO2 columns. There were large discrepancies between the CMAQ-predicted and GOME-derived NO2 columns in the fall and winter seasons. In particular, while the CMAQ-predicted NO2 columns produced larger values than the GOME-derived NO2 columns over South Korea for all four seasons, the CMAQ-predicted NO2 columns produced smaller values than the GOME-derived NO2 columns over North China for all seasons with the exception of summer (summer anomaly). It is believed that there might be some error in the NOx emission estimates as well as uncertainty in the NOx chemical loss rates over North China and South Korea. Regarding the latter, this study further focused on the biogenic VOC (BVOC) emissions that were strongly coupled with NOx chemistry during summer in East Asia. This study also investigated whether the CMAQ-modeled NO2/NOx ratios with the possibly overestimated isoprene emissions were higher than those with reduced isoprene emissions. Although changes in both the NOx chemical loss rates and NO2/NOx ratios from CMAQ-modeling with the different isoprene emissions affected the CMAQ-modeled NO2 levels, the effects were found to be limited, mainly due to the low absolute levels of NO2 in summer. Seasonal variations of the NOx emission fluxes over East Asia were further investigated by a set of sensitivity runs of the CMAQ model. Although the results still exhibited the summer anomaly possibly due to the uncertainties in both NOx-related chemistry in the CMAQ model and the GOME measurements, it is believed that consideration of both the seasonal variations in NOx emissions and the correct BVOC emissions in East Asia are critical. Overall, it is estimated that the NOx emissions are underestimated by ~57.3% in North China and overestimated by ~46.1% in South Korea over an entire year. In order to confirm the uncertainty in NOx emissions, the NOx emissions over South Korea and China were further investigated using the ACE-ASIA, REAS (Regional Emission inventory in ASia), and CAPSS (Clean Air Policy Support System) emission inventories. The comparison between the CMAQ-calculated and GOME-derived NO2 columns indicated that both the ACE-ASIA and REAS inventories have some uncertainty in NOx emissions over North China and South Korea, which can also lead to some errors in modeling the formation of ozone and secondary aerosols in South Korea and North China.


2009 ◽  
Vol 9 (2) ◽  
pp. 6363-6395 ◽  
Author(s):  
M. Zavala ◽  
S. C. Herndon ◽  
E. C. Wood ◽  
T. B. Onasch ◽  
W. B. Knighton ◽  
...  

Abstract. Mobile emissions represent a significant fraction of the total anthropogenic emissions burden in the Mexico City Metropolitan Area (MCMA) and, therefore, it is crucial to use top-down techniques informed by on-road exhaust measurements to evaluate and improve traditional bottom-up official emissions inventory (EI) for the city. We present the measurements of on-road fleet-average emission factors obtained using the Aerodyne mobile laboratory in the MCMA in March 2006 as part of the MILAGRO/MCMA-2006 field campaign. A comparison of our on-road emission measurements with those obtained in 2003 using essentially the same measurement techniques and analysis methods indicates that, in the three year span, NO emission factors remain within the measured variability ranges whereas emission factors of aldehydes and aromatics species were reduced for all sampled driving conditions. We use a top-down fuel-based approach to evaluate the mobile emissions from the gasoline fleet estimated in the bottom-up official 2006 MCMA mobile sources. Within the range of measurement uncertainties, we found probable slight overpredictions of mean EI estimates on the order of 20–28% for CO and 14–20% for NO. However, we identify a probable EI underprediction of VOC mobile emissions between 1.4 and 1.9; although estimated benzene and toluene mobile emissions in the inventory seem to be well within the uncertainties of the corresponding emissions estimates. Aldehydes mobile emissions in the inventory, however, seem to be under predicted by factors of 3 for HCHO and 2 for CH3CHO. Our on-road measurement based estimate of annual emissions of organic mass from PM1 particles suggests a severe underprediction (larger than a factor of 4) of PM2.5 mobile emissions in the inventory. Analyses of ambient CO, NOx and CO/NOx concentration trends in the MCMA indicate that the early morning ambient CO/NOx ratio has decreased at a rate of about 1.9 ppm/ppm/year over the last two decades and that the decrease has been driven by reductions in CO levels rather than by NOx concentration changes, suggesting that the relative contribution of diesel vehicles to overall NOx levels has increased over time in the city. Despite the impressive increases in the size of the vehicle fleet between 2000 and 2006, the early morning ambient concentrations of CO and NOx have not increased accordingly, probably due to the reported low removal rates of older vehicles, which do not have emissions control technologies, and partially due to the much lower emissions from newer gasoline vehicles. This indicates that an emission-based air quality control strategy targeting large reductions of emissions from mobile sources should be directed towards a significant increase of the removal rate of older, highly-polluting, vehicles.


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