scholarly journals Investigation of NO<sub>x</sub> emissions and NO<sub>x</sub>-related chemistry in East Asia using CMAQ-predicted and GOME-derived NO<sub>2</sub> columns

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.


2008 ◽  
Vol 8 (5) ◽  
pp. 17297-17341
Author(s):  
K. M. Han ◽  
C. H. Song ◽  
H. J. Ahn ◽  
C. K. Lee ◽  
A. Richter ◽  
...  

Abstract. This study examined the estimation accuracy of NOx emissions over East Asia with particular focus on North China and South Korea due to their strong source (North China)-receptor (South Korea) relationship. In order to determine contributions of North China emissions to South Korean air quality accurately, it is important to examine the accuracy of the emission inventories of both regions. 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 (receptor region) for all four seasons, the CMAQ-predicted NO2 columns produced smaller values than the GOME-derived NO2 columns over North China (source region) for all seasons with the exception of summer. It is believed that there might be some estimation error in the NOx emissions as well as large uncertainty in NOx loss rates over North China and South Korea. Regarding the latter, this study further focused on the biogenic VOC emissions that were strongly coupled with NOx chemistry in East Asia. It was found that the rates of NOx loss determined by CMAQ modeling studies might be significantly low due to the possible overestimation of biogenic isoprene emissions during summer, particularly in China. In addition, due to the possible overestimation of isoprene emissions, the CMAQ-modeled NO2/NOx ratios might show an incorrectly high level, compared with the actual NO2/NOx ratios. In addition to the retarded NOx chemical loss rates and overestimated NO2/NOx ratios, the omission of soil NOx emissions over North China during summer can lead to an underestimation of NOx emissions over North China during summer. Overall, it is estimated that the NOx emissions in North China are underestimated possibly by ~50% over an entire year. In order to confirm the uncertainty in NOx emissions, the NOx emission over South Korea was further investigated using the ACE-ASIA inventory, REAS (Regional Emission inventory in ASia) and CAPSS (Clean Air Policy Support System) by NIER (National Institute of Environmental Research) in Korea. The NOx emissions from ACE-ASIA and the REAS inventories appear to be approximately 2 times larger for mega-cities in Korea than that from the CAPSS inventory. In contrast, the NOx emissions of ACE-ASIA and REAS inventories are only 10% smaller for North China than the recently-estimated "date-back" ANL (Argonne National Laboratory) inventory. A comparison between the CMAQ-predicted and GOME-derived NO2 columns indicated that both the ACE-ASIA and REAS inventories have some uncertainty in NOx emissions over North China (A) and South Korea (C), which can lead to some error in modeling the formation of ozone and secondary aerosols in South Korea and North China.



2017 ◽  
Vol 17 (16) ◽  
pp. 10125-10141 ◽  
Author(s):  
Jieying Ding ◽  
Kazuyuki Miyazaki ◽  
Ronald Johannes van der A ◽  
Bas Mijling ◽  
Jun-ichi Kurokawa ◽  
...  

Abstract. We compare nine emission inventories of nitrogen oxides including four satellite-derived NOx inventories and the following bottom-up inventories for East Asia: REAS (Regional Emission inventory in ASia), MEIC (Multi-resolution Emission Inventory for China), CAPSS (Clean Air Policy Support System) and EDGAR (Emissions Database for Global Atmospheric Research). Two of the satellite-derived inventories are estimated by using the DECSO (Daily Emission derived Constrained by Satellite Observations) algorithm, which is based on an extended Kalman filter applied to observations from OMI or from GOME-2. The other two are derived with the EnKF algorithm, which is based on an ensemble Kalman filter applied to observations of multiple species using either the chemical transport model CHASER and MIROC-chem. The temporal behaviour and spatial distribution of the inventories are compared on a national and regional scale. A distinction is also made between urban and rural areas. The intercomparison of all inventories shows good agreement in total NOx emissions over mainland China, especially for trends, with an average bias of about 20 % for yearly emissions. All the inventories show the typical emission reduction of 10 % during the Chinese New Year and a peak in December. Satellite-derived approaches using OMI show a summer peak due to strong emissions from soil and biomass burning in this season. Biases in NOx emissions and uncertainties in temporal variability increase quickly when the spatial scale decreases. The analyses of the differences show the importance of using observations from multiple instruments and a high spatial resolution model for the satellite-derived inventories, while for bottom-up inventories, accurate emission factors and activity information are required. The advantage of the satellite-derived approach is that the emissions are soon available after observation, while the strength of the bottom-up inventories is that they include detailed information of emissions for each source category.



Atmosphere ◽  
2019 ◽  
Vol 10 (11) ◽  
pp. 658 ◽  
Author(s):  
Kyung M. Han

The study analyzed temporal variations of Ozone Monitoring Instrument (OMI)-observed NO2 columns, interregional correlation, and comparison between NO2 columns and NOx emissions during the period from 2006 to 2015. Regarding the trend of the NO2 columns, the linear lines were classified into four groups: (1) ‘upward and downward’ over six defined geographic regions in central-east Asia; (2) ‘downward’ over Guangzhou, Japan, and Taiwan; (3) ‘stagnant’ over South Korea; and (4) ‘upward’ over North Korea, Mongolia, Qinghai, and Northwestern Pacific ocean. In particular, the levels of NO2 columns in 2015 returned to those in 2006 over most of the polluted regions in China. Quantitatively, their relative changes in 2015 compared to 2006 were approximately 10%. From the interregional correlation analysis, it was found that unlike positive relationships between the polluted areas, the different variations of monthly NO2 columns led to negative relationships in Mongolia and Qinghai. Regarding the comparison between NO2 columns and NOx emission, the NOx emissions from the Copernicus Atmosphere Monitoring Service (CAMS) and Clean Air Policy Support System (CAPSS) inventories did not follow the year-to-year variations of NO2 columns over the polluted regions. In addition, the weekly effect was only clearly shown in South Korea, Japan, and Taiwan, indicating that the amounts of NOx emissions are significantly contributed to by the transportation sector.



Atmosphere ◽  
2020 ◽  
Vol 11 (1) ◽  
pp. 101 ◽  
Author(s):  
Hyun Cheol Kim ◽  
Soontae Kim ◽  
Sang-Hyun Lee ◽  
Byeong-Uk Kim ◽  
Pius Lee

Fine-scale nitrogen oxide (NOx) concentrations over South Korea are examined using surface observations, satellite data and high-resolution model simulations based on the latest emission inventory. While accurate information on NOx emissions in South Korea is crucial to understanding regional air quality in the region, consensus on the validation of NOx emissions is lacking. We investigate the spatial and temporal variation in fine-scale NOx emission sources over South Korea. Surface observations and newly available fine-scale satellite data (TROPOspheric Monitoring Instrument; TROPOMI; 3.5 × 7 km2) are compared with the community multiscale air quality (CMAQ) model based on the clean air policy support system (CAPSS) 2016 emission inventory. The results show that the TROPOMI NO2 column densities agree well with the CMAQ simulations based on CAPSS emissions (e.g., R = 0.96 for June 2018). The surface observations, satellite data and model are consistent in terms of their spatial distribution, the overestimation over the Seoul Metropolitan Area and major point sources; however, the model tends to underestimate the surface concentrations during the cold season.



2017 ◽  
Author(s):  
Jieying Ding ◽  
Kazuyuki Miyazaki ◽  
Ronald Johannes van der A ◽  
Bas Mijling ◽  
Jun-ichi Kurokawa ◽  
...  

Abstract. We compare 9 emission inventories of nitrogen oxides including four satellite-derived NOx inventories and the following bottom-up inventories for East Asia: REAS (Regional Emission inventory in ASia), MEIC (Multi-resolution Emission Inventory for China), CAPSS (Clean Air Policy Support System) and EDGAR (Emissions Database for Global Atmospheric Research). Two of the satellite-derived inventories are estimated by using the DECSO (Daily Emission derived Constrained by Satellite Observations) algorithm, which is based on an extended Kalman filter applied to observations from OMI or from GOME-2. The other two are derived with the EnKF algorithm, which is based on an ensemble Kalman Filter applied to observations of multiple species using either the chemical transport model CHASER and MIROC-chem. The temporal behaviour and spatial distribution of the inventories are compared on a national and regional scale. A distinction is also made between urban and rural areas. The intercomparison of all inventories shows good agreement in total NOx emissions over Mainland China, especially for trends, with an average bias of about 20 % for yearly emissions. All the inventories show the typical emission reduction of 10 % during the Chinese New Year and a peak in December. Satellite-derived approaches using OMI show a summer peak due to strong emissions from soil and biomass burning in this season. Biases in NOx emissions and uncertainties in temporal variability increase quickly when the spatial scale decreases. The analyses of the differences show: the importance of using observations from multiple instruments and a high spatial resolution model for the satellite-derived inventories, while for bottom-up inventories, accurate emission factors and activity information are required. The advantage of the satellite derived approach is that the emissions are soon available after observation, while the strength of the bottom-up inventories is that they include detailed information of emissions for each source category.



2020 ◽  
Vol 20 (1) ◽  
pp. 83-98 ◽  
Author(s):  
Yongjoo Choi ◽  
Yugo Kanaya ◽  
Seung-Myung Park ◽  
Atsushi Matsuki ◽  
Yasuhiro Sadanaga ◽  
...  

Abstract. The black carbon (BC) and carbon monoxide (CO) emission ratios were estimated and compiled from long-term, harmonized observations of the ΔBC∕ΔCO ratios under conditions unaffected by wet deposition at four sites in East Asia, including two sites in South Korea (Baengnyeong and Gosan) and two sites in Japan (Noto and Fukuoka). Extended spatio-temporal coverage enabled estimation of the full seasonality and elucidation of the emission ratio in North Korea for the first time. The estimated ratios were used to validate the Regional Emission inventory in ASia (REAS) version 2.1 based on six study domains (“East China”, “North China”, “Northeast China”, South Korea, North Korea, and Japan). We found that the ΔBC∕ΔCO ratios from four sites converged into a narrow range (6.2–7.9 ng m−3 ppb−1), suggesting consistency in the results from independent observations and similarity in source profiles over the regions. The BC∕CO ratios from the REAS emission inventory (7.7 ng m−3 ppb−1 for East China – 23.2 ng m−3 ppb−1 for South Korea) were overestimated by factors of 1.1 for East China to 3.0 for South Korea, whereas the ratio for North Korea (3.7 ng m−3 ppb−1 from REAS) was underestimated by a factor of 2.0, most likely due to inaccurate emissions from the road transportation sector. Seasonal variation in the BC∕CO ratio from REAS was found to be the highest in winter (China and North Korea) or summer (South Korea and Japan), whereas the measured ΔBC∕ΔCO ratio was the highest in spring in all source regions, indicating the need for further characterization of the seasonality when creating a bottom-up emission inventory. At levels of administrative districts, overestimation in Seoul, the southwestern regions of South Korea, and Northeast China was noticeable, and underestimation was mainly observed in the western regions in North Korea, including Pyongyang. These diagnoses are useful for identifying regions where revisions in the inventory are necessary, providing guidance for the refinement of BC and CO emission rate estimates over East Asia.



2017 ◽  
Author(s):  
Roger Buckley

Supported by an in-depth Introduction and contextual analysis, this six-volume set complements Series I (1918-1937 – From Armistice to North China), addressing the history between 1938 and1945. Despite the widespread operation of war-time censorship and surveillance, publishers in the West and, to a lesser degree in East Asia, put out a range of material that remains of considerable value to later generations. Some of the texts selected are undeniably partisan but the quantity of the published material (and to some extent its quality) left the general public with a vast and varied archive of printed matter that deserves to be consulted and debated by today's researchers and students. Greater attention is given to American and British literature rather than Chinese or Japanese simply by virtue of the practical realities.



2019 ◽  
Author(s):  
Yongjoo Choi ◽  
Yugo Kanaya ◽  
Seung-Myung Park ◽  
Atsushi Matsuki ◽  
Yasuhiro Sadanaga ◽  
...  

Abstract. The BC/CO emission ratios were estimated and compiled from long-term, harmonized observations of the ΔBC/ΔCO ratios under conditions unaffected by wet deposition at four sites in East Asia, including two sites in Korea (Baengnyeong and Gosan) and two sites in Japan (Noto and Fukuoka). Extended spatio-temporal coverage enabled estimation of full seasonality and elucidation of the emission ratio in North Korea, for the first time. The estimated ratios were used to validate the Regional Emission inventory in Asia (REAS) version 2.1 based on six study domains (East China, North China, Northeast China, South Korea, North Korea, and Japan). We found that the ΔBC/ΔCO ratios from four sites converged into a narrow range (6.2–7.9 ng m−3 ppb−1), suggesting consistency in the results from independent observations and similarity in source profiles over the regions. The BC/CO ratios from the REAS emission inventory (7.7 ng m−3 ppb−1 for East China – 23.2 ng m−3 ppb−1 for South Korea) were overestimated by factors of 1.1 for East China to 3.0 for South Korea, whereas the ratio for North Korea (3.7 ng m−3 ppb−1 from REAS) was underestimated by a factor of 2.0, most likely due to inaccurate emissions from the road transportation sector. Seasonal variation in the BC/CO ratio from REAS was found to be the highest in winter (China and North Korea) or summer (South Korea and Japan), whereas the measured ΔBC/ΔCO ratio was highest in spring in all source regions, indicating the need for further characterization of seasonality when creating a bottom-up emission inventory. At levels of administrative districts, overestimation in Seoul, the southwest regions of South Korea, and Northeast China was noticeable, and underestimation was mainly observed in the western regions in North Korea, including Pyongyang. These diagnoses are useful for identifying the regions where revisions in the inventory are necessary, providing guidance for refinement of BC and CO emission rate estimates over East Asia.



2018 ◽  
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.



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.



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