Global distribution of carbon monoxide
Global distribution of carbon monoxide
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DOI：
10.1029/1999jd901173
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发表时间：
2000-05-27
影响因子：
4.4
通讯作者：
Kasibhatla, P
中科院分区：
文献类型：
--
作者：
Holloway, T;Levy, H;Kasibhatla, P
本研究利用美国国家海洋和大气管理局（NOAA）地球物理流体动力学实验室三维全球化学输运模型（GFDL GCTM）探讨了一氧化碳（CO）的演化和分布。这项工作的目的是提高对全球一氧化碳收支的理解，特别关注四个来源项对CO季节变化的贡献。模型中所有CO源的总和为2.5 Pg CO/年（1 Pg = 10(3) Tg），包括化石燃料使用（300 Tg CO/年）、生物质燃烧（748 Tg CO/年）、生物烃氧化（683 Tg CO/年）和甲烷氧化（760 Tg CO/年）。CO的主要储存库是羟基自由基的破坏，我们假设羟基分布是基于Spivakovsky等人[1990]给出的三维月变化场，但我们将该场统一增加15%，以同意甲基氯仿的寿命为4.8年[Prinn等人，1995]。我们的模拟产生的一氧化碳场与NOAA/气候监测和诊断实验室全球合作烧瓶采样网络和瑞士联邦材料测试和研究实验室（EMPA）的Jungfraujoch观测站的可用测量结果（93%的季节平均数据点在+/-25%之间）和NASA全球对流层实验测量活动的飞行数据（79%的区域平均数据点）非常吻合同意在+/-25%以内)。对于所有34个地面测量站点，我们计算了每个CO源项对模式模拟的总分布的百分比贡献，并研究了这些贡献如何因运输、OH浓度变化和排放源的季节性而随季节变化。所有四种来源的CO对所有区域的CO总量都有贡献。然而，季节性通常是由化石燃料和/或生物质燃烧排放的一氧化碳的OH的运输和破坏所决定的。对羟基场的敏感性在空间上存在差异，OH产率增加30%，CO降低幅度在4-23%之间，在平流作为强局部汇的发射区附近敏感性较低。CO的寿命从夏季大陆地区的10天到冬季两极的一年多不等，我们将寿命定义为由于与OH反应而在对流层中的周转时间。
This study explores the evolution and distribution of carbon monoxide (CO) using the National Oceanic and Atmospheric Administration (NOAA) Geophysical Fluid Dynamics Laboratory three-dimensional global chemical transport model (GFDL GCTM). The work aims to gain an improved understanding of the global carbon monoxide budget, specifically focusing on the contribution of each of the four source terms to the seasonal variability of CO. The sum of all CO sources in the model is 2.5 Pg CO/yr (1 Pg = 10(3) Tg) including fossil fuel use (300 Tg CO /yr), biomass burning (748 Tg CO/yr), oxidation of biogenic hydrocarbons (683 Tg CO/yr), and methane oxidation (760 Tg CO/yr). The main sink for CO is destruction by the hydroxyl radical, and we assume a hydroxyl distribution based on three-dimensional monthly varying fields given by Spivakovsky et al. [1990], but we increase this field by 15% uniformly to agree with a methyl chloroform lifetime of 4.8 years [Prinn et al., 1995]. Our simulation produces a carbon monoxide field that agrees well with available measurements from the NOAA/Climate Monitoring and Diagnostics Laboratory global cooperative flask sampling network and from the Jungfraujoch observing station of the Swiss Federal Laboratories for Materials Testing and Research (EMPA) (93% of seasonal-average data points agree within +/-25%) and flight data from measurement campaigns of the NASA Global Tropospheric Experiment (79% of regional-average data points agree within +/-25%). For all 34 ground-based measurement sites we have calculated the percentage contribution of each CO source term to the total model-simulated distribution and examined how these contributions vary seasonally due to transport, changes in OH concentration, and seasonality of emission sources. CO from all four sources contributes to the total magnitude of CO in all regions. Seasonality, however, is usually governed by the transport and destruction by OH of CO emitted by fossil fuel and/or biomass burning. The sensitivity to the hydroxyl field varies spatially, with a 30% increase in OH yielding decreases in CO ranging from 4-23%, with lower sensitivities near emission regions where advection acts as a strong local sink. The lifetime of CO varies from 10 days over summer continental regions to well over a year at the winter poles, where we define lifetime as the turnover time in the troposphere due to reaction with OH.