scholarly journals Evaluation of anthropogenic emissions of carbon monoxide in East Asia derived from observations of atmospheric radon-222 over the Western North Pacific

2012 ◽  
Vol 12 (6) ◽  
pp. 15337-15372
Author(s):  
A. Wada ◽  
H. Matsueda ◽  
S. Murayama ◽  
S. Taguchi ◽  
A. Kamada ◽  
...  

Abstract. We used the observed CO/222Rn ratio in Asian outflows at Minamitorishima (MNM), Yonagunijima (YON), and Ryori (RYO) over the Western North Pacific from 2007 to 2011, together with a three-dimensional chemical transport model (STAG), in order to estimate anthropogenic emissions of CO in East Asia. The measurements captured high-frequency synoptic variations of enhanced 222Rn (ERN) events associated with long-range transport of continental air masses. 222Rn and CO showed high correlation during the ERN events observed at MNM and YON in the winter and spring, but not at RYO. The STAG transport model reproduced well the concentration of observed 222Rn when forced with constant and uniform flux density of 1.0 atom cm−2 s−1, but underestimated the associated enhancement of synoptically variable CO caused by the underestimated flux values in the EDGAR ver. 4.1 emission database used in the model for East Asia. Better estimates for the East Asian emission were derived using a radon tracer method based on the difference in the enhancement ratio of CO/222Rn between observation and model. The anthropogenic emission of CO for China, Japan, and Korea was estimated to be 203 Tg CO yr−1, 93% of which originated in China. When compared with other estimated emissions of CO, our estimated result showed consistency with those of the inverse method, whereas the emission database of EDGAR was about 45% smaller than our anthropogenic estimation for China.

2012 ◽  
Vol 12 (24) ◽  
pp. 12119-12132 ◽  
Author(s):  
A. Wada ◽  
H. Matsueda ◽  
S. Murayama ◽  
S. Taguchi ◽  
A. Kamada ◽  
...  

Abstract. We used the observed CO/222Rn ratio in the Asian outflows at Minamitorishima (MNM), Yonagunijima (YON), and Ryori (RYO) in the western North Pacific from 2007 to 2011, together with a three-dimensional chemical transport model (STAG), in order to estimate anthropogenic emissions of CO in East Asia. The measurements captured high-frequency synoptic variations of enhanced 222Rn (ERN) events associated with the long-range transport of continental air masses. 222Rn and CO showed high correlation during the ERN events observed at MNM and YON in the winter and spring, but not at RYO. The STAG transport model reproduced well the concentrations of observed 222Rn when forced with a constant and uniform flux density of 1.0 atom cm−2 s−1, but underestimated the associated enhancement of synoptically variable CO caused by the underestimated flux values in the EDGAR ver. 4.1 emission database used in the model for East Asia. Better estimates for the East Asian emission were derived using a radon tracer method based on the difference in the enhancement ratio of CO/222Rn between the observation and the model. The anthropogenic emissions of CO for China, Japan, and Korea were estimated to be 203 Tg CO yr−1, 91% of which originated in China. When compared with other estimated emissions of CO, our estimated result showed consistency with those of the inverse method, whereas the emission database of EDGAR was about 45% smaller than our anthropogenic estimation for China.


2006 ◽  
Vol 6 (2) ◽  
pp. 339-348 ◽  
Author(s):  
H. Fischer ◽  
M. Lawrence ◽  
Ch. Gurk ◽  
P. Hoor ◽  
J. Lelieveld ◽  
...  

Abstract. During a series of 8 measurement campaigns within the SPURT project (2001-2003), vertical profiles of CO and O3 have been obtained at subtropical, middle and high latitudes over western Europe, covering the troposphere and lowermost stratosphere up to ~14 km altitude during all seasons. The seasonal and latitudinal variation of the measured trace gas profiles are compared to simulations with the chemical transport model MATCH. In the troposphere reasonable agreement between observations and model predictions is achieved for CO and O3, in particular at subtropical and mid-latitudes, while the model overestimates (underestimates) CO (O3 in the lowermost stratosphere particularly at high latitudes, indicating too strong simulated bi-directional exchange across the tropopause. By the use of tagged tracers in the model, long-range transport of Asian air masses is identified as the dominant source of CO pollution over Europe in the free troposphere.


2011 ◽  
Vol 11 (7) ◽  
pp. 3511-3525 ◽  
Author(s):  
Y. Wang ◽  
Y. Zhang ◽  
J. Hao ◽  
M. Luo

Abstract. Both observations and a 3-D chemical transport model suggest that surface ozone over populated eastern China features a summertime trough and that the month when surface ozone peaks differs by latitude and region. Source-receptor analysis is used to quantify the contributions of background ozone and Chinese anthropogenic emissions on this variability. Annual mean background ozone over China shows a spatial gradient from 55 ppbv in the northwest to 20 ppbv in the southeast, corresponding with changes in topography and ozone lifetime. Pollution background ozone (annual mean of 12.6 ppbv) shows a minimum in the summer and maximum in the spring. On the monthly-mean basis, Chinese pollution ozone (CPO) has a peak of 20–25 ppbv in June north of the Yangtze River and in October south of it, which explains the peaks of surface ozone in these months. The summertime trough in surface ozone over eastern China can be explained by the decrease of background ozone from spring to summer (by −15 ppbv regionally averaged over eastern China). Tagged simulations suggest that long-range transport of ozone from northern mid-latitude continents (including Europe and North America) reaches a minimum in the summer, whereas ozone from Southeast Asia exhibits a maximum in the summer over eastern China. This contrast in seasonality provides clear evidence that the seasonal switch in monsoonal wind patterns plays a significant role in determining the seasonality of background ozone over China.


2015 ◽  
Vol 15 (11) ◽  
pp. 6437-6453 ◽  
Author(s):  
S. K. R. Boreddy ◽  
K. Kawamura

Abstract. In order to characterize the long-term trend of remote marine aerosols, a 12-year observation was conducted for water-soluble ions in TSP (total suspended particulate) aerosols collected from 2001 to 2012 in the Asian outflow region at Chichijima Island in the western North Pacific. We found a clear difference in chemical composition between the continentally affected and marine background air masses over the observation site. Asian continental air masses are delivered from late autumn to spring, whereas marine air masses were dominated in summer. Concentrations of non-sea salt (nss-) SO42−, NO3−, NH4+, nss-K+ and nss-Ca2+ are high in winter and spring and low in summer. On the other hand, MSA− (methanesulfonate) exhibits higher concentrations during spring and winter, probably due to springtime dust bloom or due to the direct continental transport of MSA− to the observation site. We could not find any clear decadal trend for Na+, Cl−, Mg2+ and nss-Ca2+ in all seasons, although there exists a clear seasonal trend. However, concentrations of nss-SO42− continuously decreased from 2007 to 2012, probably due to the decreased SO2 emissions in East Asia especially in China. In contrast, nss-K+ and MSA− concentrations continuously increased from 2001 to 2012 during winter and spring seasons, demonstrating that biomass burning and/or terrestrial biological emissions in East Asia are being increasingly transported from the Asian continent to the western North Pacific. This study also demonstrates that Asian dusts can act as an important source of nutrients for phytoplankton and thus sea-to-air emission of dimethyl sulfide over the western North Pacific.


2012 ◽  
Vol 12 (24) ◽  
pp. 11889-11906 ◽  
Author(s):  
G. Krysztofiak ◽  
R. Thiéblemont ◽  
N. Huret ◽  
V. Catoire ◽  
Y. Té ◽  
...  

Abstract. The SPIRALE and SWIR balloon-borne instruments were launched in the Arctic polar region (near Kiruna, Sweden, 67.9° N–21.1° E) during summer on 7 and 24 August 2009 and on 14 August 2009, respectively. The SPIRALE instrument performed in situ measurements of several trace gases including CO and O3 at altitudes between 9 and 34 km, with very high vertical resolution (∼ 5 m). The SWIR-balloon instrument measured total and partial column of several species including CO. The CO stratospheric profile from SPIRALE for 7 August 2009 shows some specific structures with large concentrations in the low levels (potential temperatures between 320 and 380 K, i.e. 10–14 km height). These structures are not present in the CO vertical profile of SPIRALE for 24 August 2009, for which the volume mixing ratios are typical from polar latitudes (∼ 30 ppb). CO total columns retrieved from the IASI-MetOp satellite sounder for the three dates of flights are used to understand this CO variability. SPIRALE and SWIR CO partial columns between 9 and 34 km are compared, allowing us to confirm that the enhancement of CO is localised in the stratosphere. The measurements are also investigated in terms of CO:O3 correlations and using several modelling approaches (trajectory calculations, potential vorticity fields, results of chemistry transport model) in order to characterize the origin of the air masses sampled. The emission sources are qualified in terms of source type (fires, urban pollution) using NH3 and CO measurements from IASI-MetOp and fires detection from MODIS on board the TERRA/AQUA satellite. The results give strong evidence that the unusual abundance of CO on 7 August is due to surface pollution plumes from East Asia and North America transporting to the upper troposphere and then entering the lower stratosphere by isentropic advection. This study strengthens evidence that the composition of low polar stratosphere in summer may be affected by anthropogenic surface emissions through long-range transport.


2005 ◽  
Vol 5 (5) ◽  
pp. 9065-9096 ◽  
Author(s):  
H. Fischer ◽  
M. Lawrence ◽  
Ch. Gurk ◽  
P. Hoor ◽  
J. Lelieveld ◽  
...  

Abstract. During a series of 8 measurement campaigns within the SPURT project (2001–2003), vertical profiles of CO and O3 have been obtained at subtropical, middle and high latitudes over western Europe, covering the troposphere and lowermost stratosphere up to ~14 km altitude during all seasons. The seasonal and latitudinal variation of the measured trace gas profiles are compared to simulations with the chemical transport model MATCH. In the troposphere reasonable agreement between observations and model predictions is achieved for CO and O3, in particular at subtropical and mid-latitudes, while the model overestimates (underestimates) CO (O3) in the lowermost stratosphere particularly at high latitudes, indicating too strong simulated bi-directional exchange across the tropopause. By the use of tagged tracers in the model, long-range transport of Asian air masses is identified as the dominant source of CO pollution over Europe in the free troposphere.


2020 ◽  
Author(s):  
Jaein Jeong ◽  
Rokjin Park ◽  
Sang-Wook Yeh ◽  
Joon-Woo Roh

<p>Interannual variability in large circulations associated with climate connections, such as monsoon and El Niño, have a significant impact on winter PM<sub>2.5</sub> concentrations in East Asia. In this study, we use the global 3D chemical transport model (GEOS-Chem) over the last 35 years to investigate the relationship between major climate variability and winter PM<sub>2.5</sub> concentrations in East Asia. First, the model is evaluated by comparing the simulated and observed aerosol concentrations with the ground and satellite-based aerosol concentrations. The results indicate that this model well reproduces the variability and magnitude of aerosol concentrations observed in East Asia. Sensitivity simulations are then used with fixed anthropogenic emissions to investigate the effects of meteorological variability on changes in aerosol concentrations in East Asia. The variability of winter PM<sub>2.5</sub> concentrations in northern East Asia was found to be closely correlated with ENSO and Siberian high position. To predict PM<sub>2.5</sub> concentrations using key climate indices, we develop multiple linear regression models. As a result, the predicted winter PM<sub>2.5</sub> concentrations using the key climate index are well reproduced in the simulated PM<sub>2.5</sub> concentrations, especially in northern East Asia.</p>


2014 ◽  
Vol 14 (8) ◽  
pp. 11177-11219 ◽  
Author(s):  
Q. Mu ◽  
H. Liao

Abstract. We used the nested grid version of the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to examine the interannual variations (IAVs) of aerosols over heavily polluted regions in China for years 2004–2012. The role of variations in meteorological parameters was quantified by a simulation with fixed anthropogenic emissions at year 2006 levels and changes in meteorological parameters over 2004–2012. Simulated PM2.5 (particles with a diameter of 2.5 μm or less) aerosol concentrations exhibited large IAVs in North China (NC, 32–42° N, 110–120° E), with regionally averaged absolute percent departure from the mean (APDM) values of 17, 14, 14, and 11% in December-January-February (DJF), March-April-May (MAM), June-July-August (JJA), and September-October-November (SON), respectively. Over South China (SC, 22–32° N, 110–120° E), the IAVs in PM2.5 were found to be the largest in JJA, with the regional mean APDM values of 14% in JJA and of about 9% in other seasons. Concentrations of PM2.5 over the Sichuan Basin (SCB, 27–33° N, 102–110° E) were simulated to have the smallest IAVs among the polluted regions examined in this work, with the APDM values of 8–9% in all seasons. All aerosol species (sulfate, nitrate, ammonium, black carbon, and organic carbon) were simulated to have the largest IAVs over NC in DJF, corresponding to the large variations in meteorological parameters over NC in this season. Process analyses were performed to identify the key meteorological parameters that determined the IAVs of different aerosol species in different regions. While the variations in temperature and specific humidity, which influenced the gas-phase formation of sulfate, jointly determined the IAVs of sulfate over NC in both DJF and JJA, wind (or convergence of wind) in DJF and precipitation in JJA were the dominant meteorological factors to influence IAVs of sulfate over SC and the SCB. The IAVs in temperature and specific humidity influenced gas-to-aerosol partitioning, which were the major factors that led to the IAVs of nitrate aerosol in China. The IAVs in wind and precipitation were found to drive the IAVs of organic carbon aerosol. We also compared the IAVs of aerosols simulated with variations in meteorological parameters alone with those simulated with variations in both meteorological parameters and anthropogenic emissions; the variations in meteorological fields were found to dominate the IAVs of aerosols in China.


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