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Sources and seasonality of atmospheric methanol based on tall tower measurements in the US Upper Midwest

机译:基于高塔测量的大气甲醇的季节性和季节性

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We present over one year (January 2010–February 2011) of continuous atmospheric methanol measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), and interpret the dataset in terms of constraints on regional methanol sources and seasonality. The seasonal cycle of methanol concentrations observed at the KCMP tall tower is generally similar to that simulated by a global 3-D chemical transport model (GEOS-Chem, driven with MEGANv2.0 biogenic emissions) except the seasonal peak occurs ~1 month earlier in the observations, apparently reflecting a model underestimate of emission rates for younger versus older leaves. Based on a source tracer approach, which we evaluate using GEOS-Chem and with multiple tracers, we estimate that anthropogenic emissions account for approximately 40% of ambient methanol abundance during winter and 10% during summer. During daytime in summer, methanol concentrations increase exponentially with temperature, reflecting the temperature sensitivity of the biogenic source, and the observed temperature dependence is statistically consistent with that in the model. Nevertheless, summertime concentrations are underestimated by on average 35% in the model for this region. The seasonal importance of methanol as a source of formaldehyde (HCHO) and carbon monoxide (CO) is highest in spring through early summer, when biogenic methanol emissions are high but isoprene emissions are still relatively low. During that time observed methanol concentrations account for on average 20% of the total CO and HCHO production rates as simulated by GEOS-Chem, compared to 12% later in the summer and 12% on an annual average basis. The biased seasonality in the model means that the photochemical role for methanol early in the growing season is presently underestimated.
机译:我们展示了一年多(2011年1月至2011年2月),从明尼苏达大学高楼轨道天然气天然气天然气天然气天然气天然气天然气观测台(KCMP高塔; 244米AGL),并以区域甲醇来源的限制来解释数据集季节性。在KCMP高塔观察到的甲醇浓度的季节性循环通常与全球3-D化学传输模型(Geos-Chem,随着Meganv2.0生物发射驱动的Geos-Chem)模拟的季节性循环通常类似于季节性峰值发生的季节性峰值〜1个月观察结果显然反映了年轻人对较旧叶子的排放率的模型。根据源示踪方法,我们使用Geos-Chem和多种示踪剂评估,我们估计人为排放占冬季冬季和10%的环境甲醇丰度的约40%。在夏季白天,甲醇浓度随温度呈指数增加,反映生物源的温度敏感性,观察到的温度依赖性与模型中的统计学上一致。尽管如此,夏季浓度平均在该地区的模型中低估了35%。甲醇作为甲醛(HCHO)和一氧化碳(CO)源的季节性重要性在春夏春季最高,当生物甲醇排放量高但异戊二烯排放仍然相对较低。在此期间,观察到的甲醇浓度平均占Geos-Chem模拟的共同综合共同股份和HCho生产率的20%,而夏季的12%和每年的12%。该模型中的偏见季节性意味着目前低估了生长季节早期甲醇的光化学作用。

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