Impacts of biomass burning in Southeast Asia on ozone and reactive nitrogen over the western Pacific in spring
Impacts of biomass burning in Southeast Asia on ozone and reactive nitrogen over the western Pacific in spring
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DOI：
10.1029/2003jd004203
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发表时间：
2004-08
影响因子：
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通讯作者：
Y. Kondo;Y. Morino;N. Takegawa;M. Koike;K. Kita;Y. Miyazaki;G. Sachse;S. Vay;M. Avery;F. F
中科院分区：
文献类型：
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作者：
Y. Kondo;Y. Morino;N. Takegawa;M. Koike;K. Kita;Y. Miyazaki;G. Sachse;S. Vay;M. Avery;F. F
[1]2001年2月至4月期间进行的太平洋上空运输和化学演变（TRACE-P）活动期间，在西太平洋上空对臭氧（O3）及其前体（活性氮、CO、非甲烷碳氢化合物）进行了飞机测量。在此期间（旱季），东南亚（SEA）的生物质燃烧活动很高，并且东南亚的对流活动经常将空气从边界层输送到自由对流层，然后向东输送到30 ° N以南的西太平洋采样区。该数据集允许从SEA流出的化学和物理过程的系统调查。氯甲烷（CH 3Cl）和CO被选为主要和次要的示踪剂，分别，以衡量从生物质燃烧的痕量物种的排放的影响程度。生物质燃烧被认为是一个主要来源的活性氮（NOx，PAN，硝酸盐）和O3在这个区域从这些物种的相关性与示踪剂。在向上运输过程中的活性氮的丰度的变化是量化的海拔变化的斜率，这些物种与CO的相关性。氮氧化物随着海拔的降低，由于其氧化为硝酸。另一方面，PAN在从对流层低层到对流层中层的传输过程中是保守的，这与其在低温下的低水溶性和化学稳定性相一致。大量的硝酸和硝酸盐，这是高度水溶性的损失，发生在自由对流层，最有可能是由于降水的湿去除。这已被证明是在对流层中部的NOy损失的主要途径。由于在SEA中的生物质燃烧的O3及其前体物的混合比的增加估计使用示踪剂。生物质燃烧直接排放的CO和总活性氮（NOy）的增加在2-4公里处最大。在这个高度上，NOy和O3的增加量分别比其背景值240 pptv和31 ppbv高出810 pptv和26 ppbv。生物质燃烧羽流中的O3-CO相关性的斜率与在澳大利亚北方、非洲和加拿大的火羽流中观察到的相似。由O3-CO斜率和NOx/CO排放比（ER）得到的O3生产效率（OPE）与C2 H4/NOx ER呈正相关，表明C2 H4/NOx ER是决定OPE的关键参数。西太平洋区域O3净通量与2004年生物质燃烧产生的O3总量的比较
[1] Aircraft measurements of ozone (O3) and its precursors (reactive nitrogen, CO, nonmethane hydrocarbons) were made over the western Pacific during the Transport and Chemical Evolution Over the Pacific (TRACE-P) campaign, which was conducted during February–April 2001. Biomass burning activity was high over Southeast Asia (SEA) during this period (dry season), and convective activity over SEA frequently transported air from the boundary layer to the free troposphere, followed by eastward transport to the sampling region over the western Pacific south of 30� N. This data set allows for systematic investigations of the chemical and physical processes in the outflow from SEA. Methyl chloride (CH3Cl) and CO are chosen as primary and secondary tracers, respectively, to gauge the degree of the impact of emissions of trace species from biomass burning. Biomass burning is found to be a major source of reactive nitrogen (NOx, PAN, HNO3, and nitrate) and O3 in this region from correlations of these species with the tracers. Changes in the abundance of reactive nitrogen during upward transport are quantified from the altitude change of the slopes of the correlations of these species with CO. NOx decreased with altitude due to its oxidation to HNO3. On the other hand, PAN was conserved during transport from the lower to the middle troposphere, consistent with its low water solubility and chemical stability at low temperatures. Large losses of HNO3 and nitrate, which are highly water soluble, occurred in the free troposphere, most likely due to wet removal by precipitation. This has been shown to be the major pathway of NOy loss in the middle troposphere. Increases in the mixing ratios of O3 and its precursors due to biomass burning in SEA are estimated using the tracers. Enhancements of CO and total reactive nitrogen (NOy), which are directly emitted from biomass burning, were largest at 2–4 km. At this altitudetheincreasesinNOyandO3were810partspertrillionbyvolume(pptv)and26parts per billion by volume (ppbv) above their background values of 240 pptv and 31 ppbv, respectively. The slope of the O3-CO correlation in biomass burning plumes was similar to those observed in fire plumes in northern Australia, Africa, and Canada. The O3 production efficiency (OPE) derived from the O3-CO slope and NOx/CO emission ratio (ER) is shown to be positively correlated with the C2H4/NOx ER, indicating that the C2H4/NOx ER is a critical parameter in determining the OPE. Comparison of the net O3 flux across the western Pacific region and total O3 production due to biomass burning in