Relationship between long-range transported atmospheric black carbon and carbon monoxide at a high-altitude background station in East Asia

2019 ◽  
Vol 210 ◽  
pp. 86-99 ◽  
Author(s):  
Shantanu Kumar Pani ◽  
Chang-Feng Ou-Yang ◽  
Sheng-Hsiang Wang ◽  
John A. Ogren ◽  
Patrick J. Sheridan ◽  
...  
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):  
Kohei Ikeda ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Hideharu Akiyoshi ◽  
Yugo Kanaya ◽  
...  

Abstract. We implemented a tagged tracer method of black carbon (BC) into a global chemistry-transport model GEOS-Chem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and found that the simulated seasonal variations were improved by implementing an aging parameterization and reducing the wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62 % to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Okhotsk Sea and East Siberia during winter and spring. We identified an important window area, which allowed a strong incoming of East Asian BC to the Arctic (130°–180° E and 3–8 km altitude at 66° N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km altitude due to uplifting during the long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was smaller than that from other large source regions such as Europe, Russia and North America. However, the East Asian contribution was most important for BC in the middle troposphere (41 %) and BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of the Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12–15 %, which became the maximum during summer.


2011 ◽  
Vol 11 (18) ◽  
pp. 9735-9747 ◽  
Author(s):  
X. L. Pan ◽  
Y. Kanaya ◽  
Z. F. Wang ◽  
Y. Liu ◽  
P. Pochanart ◽  
...  

Abstract. Understanding the relationship between black carbon (BC) and carbon monoxide (CO) will help improve BC emission inventories and the evaluation of global/regional climate forcing effects. In the present work, the BC (PM1) mass concentration and CO mixing ratio were continuously measured at a high-altitude background station on the summit of Mt. Huang (30.16° N, 118.26° E, 1840 m a.s.l.). Annual mean BC mass concentration was 1004.5 ± 895.5 ng m−3 with maxima in spring and autumn, and annual mean CO mixing ratio was 424.1 ± 159.2 ppbv. A large increase of CO was observed in the cold season, implying the contribution from the large-scale domestic coal/biofuel combustion for heating. The BC-CO relationship was found to show different seasonal features but strong positive correlation (R>0.8). In Mt. Huang area, the ΔBC/ΔCO ratio showed unimodal diurnal variations and had a maximum during the day (09:00–17:00 LST) and minimum at night (21:00–04:00 LST) in all seasons, indicating the impact of planetary boundary layer and the intrusion of clean air masses from the high troposphere. Back trajectory cluster analysis showed that the ΔBC/ΔCO ratio of plumes from the Eastern China (Jiangsu, Zhejiang provinces and Shanghai) was 8.8 ± 0.9 ng m−3 ppbv−1. Transportation and industry were deemed as controlling factors of the BC-CO relationship in this region. The ΔBC/ΔCO ratios for air masses from Northern China (Anhui, Henan, Shanxi and Shandong provinces) and southern China (Jiangxi, Fujian and Hunan provinces) were quite similar with mean values of 6.5 ± 0.4 and 6.5 ± 0.2 ng m−3 ppbv−1 respectively. The case studies combined with satellite observations demonstrated that the ΔBC/ΔCO ratio for biomass burning (BB) plumes were 10.3 ± 0.3 and 11.6 ± 0.5ng m−3 ppbv−1, significantly higher than those during non-BB impacted periods. The loss of BC during transport was also investigated on the basis of the ΔBC/ΔCO-RH (relative humidity) relationship along air mass pathways. The results showed that BC particles from Eastern China area was much more easily removed from atmosphere than other inland regions due to the higher RH along transport pathway, implying the importance of chemical compositions and mixing states on BC residence time in the atmosphere.


2011 ◽  
Vol 11 (2) ◽  
pp. 4447-4485 ◽  
Author(s):  
X. L. Pan ◽  
Y. Kanaya ◽  
Z. F. Wang ◽  
Y. Liu ◽  
P. Pochanart ◽  
...  

Abstract. Understanding the relationship between black carbon (BC) and carbon monoxide (CO) will help improve BC emission inventories and the evaluation of global/regional climate forcing effects. In the present work, the BC (PM1) and CO mixing ratio was continuously measured at a~high-altitude background station on the summit of Mt Huangshan between 2006 and 2009. Annual mean BC concentration was 654.6 ± 633.4 ng m−3 with maxima in spring and autumn, when biomass was burned over a large area in Eastern China. The yearly averaged CO concentration was 446.4 ± 167.6 ppbv, and the increase in the CO concentration was greatest in the cold season, implying that the large-scale domestic coal/biofuel combustion for heating has an effect. The BC–CO relationship was found to have different seasonal features but strong positive correlation (R > 0.8). Back trajectory cluster analysis showed that the ΔBC/ΔCO ratio of plumes from the Yangtze River Delta region was 6.58 ± 0.96 ng m−3 ppbv−1, which is consistent with result from INTEX-B emission inventory. The ΔBC/ΔCO ratios for air masses from Northern, Central Eastern and Southern China were 5.2 ± 0.63, 5.65 ± 0.58 and 5.21 ± 0.93 ng m−3 ppbv−1, respectively. Over the whole observation period, the ΔBC/ΔCO ratio had unimodal diurnal variations and had a maximum during the day (09:00–17:00 LST) and minimum at night (21:00–04:00 LST) in spring, summer, autumn and winter, indicating the effects of the intrusion of clean air mass from the high troposphere. The case study combined with measurements of urban PM10 concentrations and satellite observations demonstrated that the ΔBC/ΔCO ratio for a plume of burning biomass was 12.4 ng m−3 ppbv−1 and that for urban plumes in Eastern China was 5.3 ± 0.53 ng m−3 ppbv−1. Transportation and industry were deemed as controlling factors of the BC–CO relationship and major contributions to atmospheric BC and CO loadings in urban areas. The loss of BC during transportation was also investigated on the basis of the ΔBC/ΔCO–RH relationship along air mass pathways, and the results showed that 30–50% BC was lost when air mass traveled under higher RH conditions (>60%) for 2 days.


2014 ◽  
Vol 14 (8) ◽  
pp. 4279-4295 ◽  
Author(s):  
A. Ripoll ◽  
J. Pey ◽  
M. C. Minguillón ◽  
N. Pérez ◽  
M. Pandolfi ◽  
...  

Abstract. Time variation of mass particulate matter (PM1 and PM1&minus10), black carbon (BC) and number of particles (N3: number of particles with an aerodynamic diameter higher than 3 nm, and N10: higher than 10 nm) concentrations at the high-altitude site of Montsec (MSC) in the southern Pyrenees was interpreted for the period 2010–2012. At MSC, PM10 (12 μg m−3) and N7 (2140 # cm−3) three-year arithmetic average concentrations were higher than those measured at other high-altitude sites in central Europe during the same period (PM10: 3–9 μg m−3 and N: 634–2070 # cm−3). By contrast, BC concentrations at MSC (0.2 μg m−3) were equal to or even lower than those measured at these European sites (0.2–0.4 μg m−3). These differences were attributed to the higher relevance of Saharan dust transport and to the higher importance of the biogenic precursor emissions and new particle formation (NPF) processes, and to the lower influence of anthropogenic emissions at MSC. The different time variation of PM and BC concentrations compared with that of N suggests that these aerosol parameters were governed by diverse factors at MSC. Both PM and BC concentrations showed marked differences for different meteorological scenarios, with enhanced concentrations under North African air outbreaks (PM1&minus10: 13 μg m−3, PM1: 8 μg m−3 and BC: 0.3 μg m−3) and low concentrations when Atlantic advections occurred (PM1−10: 5 μg m−3, PM1: 4 μg m−3 and BC: 0.1 μg m−3). PM and BC concentrations increased in summer, with a secondary maximum in early spring, and were at their lowest in winter, due to the contrasting origin of the air masses in the warmer seasons (spring and summer) and in the colder seasons (autumn and winter). The maximum in the warmer seasons was attributed to long-range transport processes that mask the breezes and regional transport breaking the daily cycles of these pollutants. By contrast, PM and BC concentrations showed clear diurnal cycles, with maxima at midday in the colder seasons. A statistically significant weekly variation was also obtained for the BC concentrations, displaying a progressive increase from Tuesday to Saturday, followed by a significant decrease on Sunday and Monday. N concentrations depended more on local meteorological variables such as temperature and solar radiation intensity than on the origin of the air mass. Therefore, arithmetic averages as a function of meteorological episodes showed the highest concentrations of N during summer regional episodes (N3: 4461 # cm−3 and N7: 3021 # cm−3) and the lowest concentrations during winter regional scenarios (N3: 2496 # cm−3 and N7: 1073 # cm−3). This dependence on temperature and solar radiation also accounted for the marked diurnal cycle of N concentrations throughout the year, with a peak at midday and for the absence of a weekly pattern. Measurements carried out at MSC enabled us to characterize the tropospheric background aerosols in the western Mediterranean basin (WMB). Our results highlight the importance of the NPF processes in southern Europe, underline the high contribution of long-range dust transport with respect to central Europe and its prevalence in elevated layers, and reveal that MSC is much less affected by anthropogenic emissions than other high-altitude sites in central Europe.


2017 ◽  
Vol 17 (17) ◽  
pp. 10515-10533 ◽  
Author(s):  
Kohei Ikeda ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Hideharu Akiyoshi ◽  
Yugo Kanaya ◽  
...  

Abstract. We implemented a tagged tracer method of black carbon (BC) into a global chemistry transport model, GEOS-Chem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and examined the sensitivity of an aging parameterization and wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62 % to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Sea of Okhotsk and eastern Siberia during winter and spring. We identified an important window area, which allowed a strong incoming of East Asian BC to the Arctic (130–180° E and 3–8 km of altitude at 66° N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km of altitude due to uplifting during long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was lower than that from other large source regions such as Europe, Russia, and North America. However, the East Asian contribution was the most important for BC in the middle troposphere (41 %) and the BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska, and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12–15 %, which became the maximum during summer.


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