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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.
Atmospheric Chemistry and Physics Discussions. 01/2011;
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Yamaji K,
Li J,
Uno I,
Kanaya Y,
Irie H,
Takigawa M,
Komazaki Y, Pochanart P,
Liu Y,
Tanimoto H,
Ohara T,
Yan X,
Wang Z,
Akimoto H
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ABSTRACT: The impact of open crop residual burning (OCRB) on O3, CO, black carbon (BC) and organic carbon (OC) concentrations over Central Eastern China (CEC; 30–40° N, 111–120° E), during the Mount Tai Experiment in 2006 (MTX2006) was evaluated using a regional chemical transport model, the Models–3 Community Multiscale Air Quality Modeling System (CMAQ). To investigate these pollutants during MTX2006 in June 2006, daily gridded OCRB emissions were developed based on a bottom-up methodology using land cover and hotspot information from satellites. This model system involving daily emissions captured monthly–averages of observed concentrations and day-to-day variations in the patterns of O3, CO, BC and OC at the summit of Mount Tai (36° N, 117° E, 1534 m a.s.l., Shandong Province of the People's Republic of China) with high correlation coefficients between the model and observations ranging from 0.55 to 0.69. These results were significantly improved from those using annual biomass burning emissions. For monthly-averaged O3, the simulated concentration of 80.8 ppbv was close to the observed concentration (81.3 ppbv). The MTX2006 period was roughly divided into two parts: 1) polluted days with heavy OCRB in the first half of June; and 2) cleaner days with negligible field burning in the latter half of June. Additionally, the first half of June was characterized by two high-pollution episodes during 5–7 and 12–13 June, separated by a relatively cleaner intermediate period during 8–10 June. In the first high-pollution episode, the model captured the high O3, CO, BC and OC concentrations at the summit of Mount Tai, which were associated with OCRB over southern CEC and subsequent northward transport. For this episode, the impacts of OCRB emissions on pollutant concentrations were 26% (O3), 62% (CO), 79% (BC) and 80% (OC) at the summit of Mount Tai. The daily OCRB emissions were an essential factor in the evaluation of these pollutants during MTX2006. These emissions have a large impact not only on primary pollutants but also on secondary pollutants, such as O3, in the first half of June over northeastern Asia. The model reproduced reasonably well the variation of these pollutants in MTX2006, but underestimated daily averages of both CO and BC by a factor of 2, when using emission data from almost solely anthropogenic fuel sources in the latter half of the observation period when field burning can be neglected.
Atmospheric Chemistry and Physics. 01/2010;
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ABSTRACT: The measurement of volatile organic compounds (VOCs) was carried out at the summit of Mount Tai, located in the center of the Central East China (CEC) region, in June 2006 as part of the Mount Tai Experiment 2006 (MTX2006), which focused on the ozone and aerosol chemistry in the region. Temporal variations of simple VOCs between 2 June and 28 June revealed the characteristics of an aged air mass with minimum local influence. A comparison of VOCs observed at Mount Tai with other Chinese sites revealed relatively similar VOC levels to remote sites and, as expected, a lower level compared to more polluted sites. However, relatively high acetylene and benzene levels at Mount Tai were evidently indicated from comparison with normalized VOC profile by ethane suggested for Beijing. Owing to a shift in boundary layer height, we observed considerable differences between daytime and nighttime VOC mixing ratios. This suggests that the site potentially has a very useful characteristic of being able to measure regional polluted air and the free troposphere regional background air quality. Influence of emissions from biomass burning in the region was evidently found to be extensive during the first half of the campaign (2–15 June), using fire spot data coupling with backward trajectory analysis. Agricultural residue burning was suggested as the primary source of emissions elucidated by the slope of the correlation plot between CH3Cl and CO obtained during the first half of the campaign.
Atmospheric Chemistry and Physics. 01/2010;
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ABSTRACT: Owing to recent industrialization, Central East China has become a significant source of air pollutants. To examine the processes controlling the chemistry and transport of tropospheric ozone, we continuously measured non-methane volatile organic compounds (NMVOCs) as part of an intensive field campaign at Mount Tai, China, in June 2006 (MTX2006), using proton transfer reaction mass spectrometry (PTR-MS). Temporal variations of NMVOCs were recorded in mass-scan mode from m/z 17 to m/z 300 during 12–30 June 2006. More than thirty kinds of NMVOCs were detected up to m/z 160, including alkenes, aromatics, alcohols, aldehydes, and ketones. Oxygenated VOCs were the predominant NMVOCs. During the night of 12 June, we observed an episode of high NMVOCs concentrations attributed to the burning of agricultural biomass. The ΔNMVOCs/ΔCO ratios derived by PTR-MS measurements for this episode are compared to emission ratios from various types of biomass burning as reviewed by Andreae and Merlet (2001) and to ratios recently measured by PTR-MS in tropical forests (Karl et al., 2007) and at urban sites (Warneke et al., 2007).
Atmospheric Chemistry and Physics Discussions. 01/2009;
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Kanaya Y, Pochanart P,
Liu Y,
Li J,
Tanimoto H,
Kato S,
Suthawaree J,
Inomata S,
Taketani F,
Okuzawa K,
Kawamura K,
Akimoto H,
Z. F. Wang
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ABSTRACT: An observation-based box model approach was undertaken to estimate concentrations of OH, HO2, and RO2 radicals and the net photochemical production rate of ozone at the top of Mount Tai, located in the middle of Central East China, in June 2006. The model calculation was constrained by the measurements of O3, H2O, CO, NO, NO2, hydrocarbon, HCHO, and CH3CHO concentrations, and temperature and J values. The net production rate of ozone was estimated to be 6.4 ppb h−1 as a 6-h average (09:00–15:00 CST), suggesting 58 ppb of ozone is produced in one day. Thus the daytime buildup of ozone recorded at the mountain top as 23 ppb on average is likely affected by in situ photochemistry as well as by the upward transport of polluted air mass in the daytime. On days with high ozone concentrations (hourly values exceeding 100 ppb at least once), in situ photochemistry was more active than it was on low ozone days, suggesting that in situ photochemistry is an important factor controlling ozone concentrations. Sensitivity model runs for which different NOx and hydrocarbon concentrations were assumed suggested that the ozone production occurred normally under NOx-limited conditions, with some exceptional periods (under volatile-organic-compound-limited conditions) in which there was fresh pollution. We also examined the possible influence of the heterogeneous loss of gaseous HO2 radicals in contact with aerosol particle surfaces on the rate and regimes of ozone production.
Atmospheric Chemistry and Physics Discussions. 01/2009;
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Yamaji K,
Li J,
Uno I,
Kanaya Y,
Komazaki Y, Pochanart P,
Liu Y,
Takigawa M,
Ohara T,
Yan X,
Wang Z,
Akimoto H
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ABSTRACT: The impact of open crop residual burning on O3, CO, Black Carbons (BC), and Organic Carbons (OC) concentrations over Central Eastern China (CEC) during the Mount Tai Experiment 2006 (MTX2006) was evaluated using the regional chemical transport model, the Models-3 Community Multiscale Air Quality Modeling System (CMAQ). To investigate these pollutants during the MTX2006 period in June, daily gridded emissions from open crop residual burning were developed based on a bottom-up methodology and using land cover and hotspot information from satellites. This model system which involves daily emissions from open biomass burning, captured monthly-averaged observed concentrations and day-to-day variations in the patterns of O3, CO, BC, and OC with good correlation coefficients between models and observations, ranging from 0.54 to 0.66. These results were significantly improved from those using annual emissions. For monthly-averaged O3, the simulated concentration of 81.5 ppbv was close to the observed concentration (82.5 ppbv). The period of MTX2006 was roughly divided into two parts: 1) polluted days with heavy open crop residual burning in the first half of June; 2) cleaner days with negligible field burning in the latter half of June. Additionally, the first half of June was defined by two high pollution episodes during 5–7 and 12–13 June, and a relatively cleaner episode during 8–10 June between these two high pollution episodes. In the first polluted episode, this model captured high O3, CO, BC, and OC concentrations at the summit of Mount Tai which were affected by open crop residual burning in the south of CEC and northward transport. For this episode, the impacts from open crop residual burning were 12% for O3, 35% for CO, 56% for BC, and 80% for OC over CEC. The daily emissions from open crop residual burning were an essential factor to evaluate the pollutants during the MTX2006. These emissions have a large impact not only on primary pollutants but also on secondly pollutions, such as O3, in the first half of June over northeastern Asia. On the other hand, this model did not capture the second polluted episode and underestimated observed CO and BC. Improvements of both anthropogenic and open burning emissions and CO inflow from model boundary are necessary to improve both anthropogenic and open burning emissions and CO inflow to evaluate the pollutants using this model.
Atmospheric Chemistry and Physics Discussions. 01/2009;
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ABSTRACT: To better understand the contribution of biogenic volatile organic compounds to the formation of secondary organic aerosol (SOA) in high mountain regions, ambient aerosols were collected at the summit of Mt. Tai (1534 m, a.s.l.), Central East China (CEC) during the Mount Tai eXperiment 2006 campaign (MTX2006) in early summer. Biogenic SOA tracers of isoprene, monoterpenes, and β-caryophyllene oxidation products were measured using gas chromatography/mass spectrometry. All the biogenic SOA tracers showed no clear diurnal variations, suggesting that they are formed during long-range atmospheric transport. Although isoprene- and monoterpene-derived SOA tracers did not correlate with levoglucosan (a biomass burning tracer), β-caryophyllinic acid showed a good correlation with levoglucosan, indicating that biomass burning may be a source for this compound. Total concentrations of isoprene oxidation products are much higher than those of monoterpene and β-caryophyllene oxidation products. The ratio of isoprene to monoterpene oxidation products (Riso/mono) was found to co-vary with ozone and NOx during the summer campaign. The average Riso/mono value was 6.94 at daytime and 10.0 at nighttime. These values are among the highest in the aerosols studied in different regions, which may be due to the large isoprene fluxes, high O3 and NOx levels and relatively high OH concentrations in CEC. Using a tracer-based method, we estimated the average concentrations of secondary organic carbon (SOC) derived from isoprene, monoterpenes, and β-caryophyllene to be 1.76 μgC m−3 at daytime and 1.85 μgC m−3 at nighttime. These values correspond to 11.2% and 11.0% of the total OC concentrations, in which isoprene-derived SOC are 7.4% and 8.0% at day- and night-time, respectively. This study suggests that isoprene is a more significant precursor for biogenic SOA than monoterpenes and β-caryophyllene in high altitude in CEC.
Atmospheric Chemistry and Physics Discussions. 01/2009;
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ABSTRACT: A 3-D regional chemical transport model, the Nested Air Quality Prediction Model System (NAQPMS), with an on-line tracer tagging module was used to study the source of the near-ground (3 over CEC. The regional-scale transport of pollutants also played an important role in the spatial and temporal distribution of ozone over CEC. Chemically produced ozone from the southern part of the study region can be transported northeastwardly to the northern rim of CEC; the mean contribution was 5–10 ppbv, and it reached 25 ppbv during high ozone events. Studies of the outflow of CEC ozone and its precursors, as well as their influences and contributions to the ozone level over adjacent regions/countries, revealed that the contribution of CEC ozone to mean ozone mixing ratios over the Korean Peninsula and Japan was 5–15 ppbv, of which about half was due to the direct transport of ozone from CEC and half was produced locally by ozone precursors transported from CEC.
Atmospheric Chemistry and Physics. 01/2008;
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ABSTRACT: The impact of the East Asia monsoon on the seasonal behavior of O3 in the boundary layer of Eastern China and the west Pacific region was analyzed for 2004–2006 by means of full-year nested chemical transport model simulations and continuous observational data obtained from three inland mountain sites in central and eastern China and three oceanic sites in the west Pacific region. The basic common features of O3 seasonal behaviors over all the monitoring sites are the pre- and post-monsoon peaks with a summer trough. Such bimodal seasonal patterns of O3 are predominant over the region with strong summer monsoon penetration, and become weaker or even disappear outside the monsoon region. The seasonal/geographical distribution of the pre-defined Monsoon Index indicated that the East Asia summer monsoon is responsible for the bimodal seasonal O3 pattern, and also partly account for the differences in the O3 seasonal variations between the inland mountain and oceanic sites. Over the inland mountain sites, the O3 concentration increased gradually from the beginning of the year, reached a maximum in June, decreased rapidly to a minimum in July or August, and then peaked in September or October, thereafter decreased gradually again. Over the oceanic sites, O3 abundance showed a similar increasing trend beginning in January, but then decreased gradually from the end of March, followed by a wide trough with the minimum in July and August and a small peak in October or November. A sensitivity analysis performed by setting China-emission to zero revealed that the chemically produced O3 from China-emission contributed more than 40% of total boundary layer O3 during summertime (60–70% in June) and accounted for about 40 ppb of each peak value over the inland region. In contrast, over the oceanic region in the high monsoon index zone, the contribution of China-emission to total O3 was always less than 20% (<10 ppb), and less than 10% in summer.
Atmospheric Chemistry and Physics Discussions. 01/2008;
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ABSTRACT: Mass concentrations of black carbon (BC) were determined in June 2006 at the top of Mount Tai (36.26° N, 117.11° E, 1534 m a.s.l.), located in the middle of Central East China, using four different instruments: a multi-angle absorption photometer (5012 MAAP, Thermo), a particle soot absorption photometer (PSAP, Radiance Research), an ECOC semi-continuous analyzer (Sunset Laboratory) and an Aethalometer (AE-21, Magee Scientific). High correlation coefficients (R2>0.88) were obtained between the measurements of the BC mass concentrations by the different instruments. From the range of the slopes of the linear least-square fittings, we concluded that the BC concentrations regionally-representative of the area were measured in a range with a maximum-to-minimum ratio of 1.5 (an exception was that the BC (PM2.5) concentrations derived from MAAP were ~2 times higher than the optical measurements (PM2.5) derived from the ECOC analyzer). This range is significant, but is still sufficiently narrow to better constrain the large and highly uncertain emission rate of BC from China. In detail, two optical instruments (the MAAP instrument and the PSAP instrument equipped with a heated inlet (400°C)) tended to give higher concentrations than the thermal EC concentrations observed by the ECOC analyzer. The ratios of optical BC to thermal EC showed a positive correlation with the OC/EC ratio reported by the ECOC analyzer, suggesting two possibilities. One is that the optical instruments overestimated BC concentrations in spite of careful cancellation of the scattering effect in the MAAP instrument and the expected evaporation of volatile species by heating the inlet of the PSAP instrument. The other is that the determined split points between OC and EC were too late when a large amount of OC underwent charring during the analysis, resulting in an underestimation of EC by the ECOC analyzer. High ratios of optical BC to thermal EC were recorded when the NOx/NOy ratio was low, implying the coating of the particles became thicker in the aged air mass and resulted in the optical instruments overestimating BC concentrations owing to the lensing effect.
Atmospheric Chemistry and Physics Discussions. 01/2008;
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ABSTRACT: A 3-D regional chemical transport model, the Nested Air Quality Prediction Model System (NAQPMS), with an on-line tracer tagging module was applied to study the source of the near-ground (3 over CEC is controlled by the photochemical reactions. In addition, the regional-scale transport of pollutants also plays an important role in the spatial and temporal distribution of ozone over CEC. The chemically produced ozone from the southern part of the study region can be transported northeastwardly to the northern rim of CEC. The mean contribution is 5–10 ppbv, and it can reach 25 ppbv during high ozone events. This work also studied the outflow of CEC ozone and its precursors, as well as their influences and contributions to the ozone level over adjacent regions/countries. It shows that the contribution of CEC ozone to mean ozone mixing ratios over Korea Peninsula and Japan is 5–15 ppbv, of which about half was due to the direct transport of ozone from CEC and half was contributed by the ozone produced locally by the transported ozone precursors from CEC.
Atmospheric Chemistry and Physics Discussions. 01/2008;
