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Factors controlling black carbon distribution in the Arctic

机译:控制北极黑碳分布的因素

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We investigate the sensitivity of black carbon (BC) in the Arctic, including BC concentration in snow (BCsnow, ng?g?1) and surface air (BCair, ng?m?3), as well as emissions, dry deposition, and wet scavenging using the global three-dimensional (3-D) chemical transport model (CTM) GEOS-Chem. We find that the model underestimates BCsnow in the Arctic by 40?% on average (median??=??11.8?ng?g?1). Natural gas flaring substantially increases total BC emissions in the Arctic (by ~?70?%). The flaring emissions lead to up to 49?% increases (0.1–8.5?ng?g?1) in Arctic BCsnow, dramatically improving model comparison with observations (50?% reduction in discrepancy) near flaring source regions (the western side of the extreme north of Russia). Ample observations suggest that BC dry deposition velocities over snow and ice in current CTMs (0.03?cm?s?1 in the GEOS-Chem) are too small. We apply the resistance-in-series method to compute a dry deposition velocity (vd) that varies with local meteorological and surface conditions. The resulting velocity is significantly larger and varies by a factor of 8 in the Arctic (0.03–0.24?cm?s?1), which increases the fraction of dry to total BC deposition (16 to 25?%) yet leaves the total BC deposition and BCsnow in the Arctic unchanged. This is largely explained by the offsetting higher dry and lower wet deposition fluxes. Additionally, we account for the effect of the Wegener–Bergeron–Findeisen (WBF) process in mixed-phase clouds, which releases BC particles from condensed phases (water drops and ice crystals) back to the interstitial air and thereby substantially reduces the scavenging efficiency of clouds for BC (by 43–76?% in the Arctic). The resulting BCsnow is up to 80?% higher, BC loading is considerably larger (from 0.25 to 0.43?mg?m?2), and BC lifetime is markedly prolonged (from 9 to 16?days) in the Arctic. Overall, flaring emissions increase BCair in the Arctic (by ~?20?ng?m?3), the updated vd more than halves BCair (by ~?20?ng?m?3), and the WBF effect increases BCair by 25–70?% during winter and early spring. The resulting model simulation of BCsnow is substantially improved (within 10?% of the observations) and the discrepancies of BCair are much smaller during the snow season at Barrow, Alert, and Summit (from ?67–?47?% to ?46–3?%). Our results point toward an urgent need for better characterization of flaring emissions of BC (e.g., the emission factors, temporal, and spatial distribution), extensive measurements of both the dry deposition of BC over snow and ice, and the scavenging efficiency of BC in mixed-phase clouds. In addition, we find that the poorly constrained precipitation in the Arctic may introduce large uncertainties in estimating BCsnow. Doubling precipitation introduces a positive bias approximately as large as the overall effects of flaring emissions and the WBF effect; halving precipitation produces a similarly large negative bias.
机译:我们研究了北极的黑碳(BC)的敏感性,包括雪中的BC浓度(BCSNow,NG?G?1)和表面空气(Bcair,Ng?M?3),以及排放,干燥沉积和使用全球三维(3-D)化学传输模型(CTM)Geos-Chem的湿扫。我们发现该模型低估了北极的BCSNow平均40?%(中位数?? = ?? 11.8?G?1)。天然气辐射大大增加了北极(〜〜70?%)中的总BC排放量。燃烧的排放导致北极BCSNow中的增加(0.1-8.5?Ng?1),大大改善了与辐射源区附近的观察(差异50倍)的观察(50?%)的模型比较俄罗斯的极端北部)。充足的观察结果表明,在当前CTMS中的冰雪和冰上的BC干沉积速度(0.03?cm 2在Geos-chem)的冰上太小。我们应用串联的抗性方法来计算随着局部气象和表面条件而变化的干燥沉积速度(VD)。得到的速度显着较大,在北极(0.03-0.24Ω·cm =s≤1)中的8倍,这增加了干燥至总BC沉积的一部分(16至25μl)但留下了总BC沉积和BCSNow在北极不变。这主要通过偏移较高的干燥和较低的湿沉积通量来解释。此外,我们考虑了Wegener-Bergeron-Findeisen(WBF)过程在混合相云中的影响,该过程将来自浓缩阶段(水滴和冰晶)释放回间质空气的BC颗粒,从而大大降低了清除效率BC的云(北极中43-76?%)。得到的BCSNow较高高达80倍,BC负载量显着较大(从0.25至0.43Ω·mg?M≥2),并且BC寿命在北极地区延长(从9至16?天)。总体而言,喇叭形排放增加了北极的Bcair(〜?20?ng?m?3),更新的Vd超过一半bcair(by〜?20?ng?m?3),并且wbf效果增加bcair 25冬季和早春期间%的人。 BCSNow的所得模型模拟基本上改善(在观察中的10℃内),Bcair的差异在Barrow,警报和峰会上的雪季(来自?67-?47?%到?46- 3?%)。我们的结果迫切需要更好地表征BC的发出辐射排放(例如,排放因子,时间和空间分布),广泛测量BC在雪和冰上的干燥沉积,以及BC的清除效率混合相云。此外,我们发现北极的受损沉积不良可能会引入估计BCSNow的巨大不确定性。加倍降水引入正面偏差大致大,作为喇叭形排放和WBF效应的整体影响;减少降水产生类似的负面偏差。

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