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修订挥发性有机化合物(VOC)排放物种组成可改善全球背景乙烷和丙烷的模拟。

Revising VOC emissions speciation improves the simulation of global background ethane and propane.

作者信息

Rowlinson Matthew J, Evans Mat J, Carpenter Lucy J, Read Katie A, Punjabi Shalini, Adedeji Adedayo, Fakes Luke, Lewis Ally, Richmond Ben, Passant Neil, Murrells Tim, Henderson Barron, Bates Kelvin H, Helmig Detlev

机构信息

National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK.

Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK.

出版信息

Atmos Chem Phys. 2024 Jul 24;24(14):8317-8342. doi: 10.5194/acp-24-8317-2024.

Abstract

Non-Methane Volatile Organic Compounds (NMVOCs) generate ozone (O) when they are oxidized in the presence of oxides of nitrogen, modulate the oxidative capacity of the atmosphere and can lead to the formation of aerosol. Here, we assess the capability of a chemical transport model (GEOS-Chem) to simulate NMVOC concentrations by comparing ethane, propane and higher alkane observations in remote regions from the NOAA Flask Network and the World Meteorological Organization's Global Atmosphere Watch (GAW) network. Using the Community Emissions Data System (CEDS) inventory we find a significant underestimate in the simulated concentration of both ethane (35%) and propane (64%), consistent with previous studies. We run a new simulation where the total mass of anthropogenic NMVOC emitted in a grid box is the same as that used in CEDS, but with the NMVOC speciation derived from regional inventories. For US emissions we use the National Emissions Inventory (NEI), for Europe we use the UK National Atmospheric Emissions Inventory (NAEI), and for China, the Multi-resolution Emission Inventory for China (MEIC). These changes lead to a large increase in the modelled concentrations of ethane, improving the mean model bias from -35% to -4%. Simulated propane also improves (from -64% to -48% mean model bias), but there remains a substantial model underestimate. There were relatively minor changes to other NMVOCs. The low bias in simulated global ethane concentration is essentially removed, resolving one long-term issue in global simulations. Propane concentrations are improved but remain significantly underestimated, suggesting the potential for a missing global propane source. The change in the NMVOC emission speciation results in only minor changes in tropospheric O and OH concentrations.

摘要

非甲烷挥发性有机化合物(NMVOCs)在氮氧化物存在下被氧化时会生成臭氧(O),调节大气的氧化能力,并可能导致气溶胶的形成。在此,我们通过比较美国国家海洋和大气管理局(NOAA)气样采集网以及世界气象组织全球大气观测网(GAW)在偏远地区的乙烷、丙烷和高级烷烃观测数据,评估化学传输模型(GEOS-Chem)模拟NMVOC浓度的能力。利用社区排放数据系统(CEDS)清单,我们发现模拟的乙烷浓度(35%)和丙烷浓度(64%)均被显著低估,这与之前的研究一致。我们进行了一项新的模拟,其中网格箱中人为排放的NMVOC总质量与CEDS中使用的相同,但NMVOC的物种组成源自区域清单。对于美国的排放,我们使用国家排放清单(NEI),对于欧洲,我们使用英国国家大气排放清单(NAEI),对于中国,我们使用中国多分辨率排放清单(MEIC)。这些变化导致模拟的乙烷浓度大幅增加,将模型平均偏差从-35%改善至-4%。模拟的丙烷浓度也有所改善(从-64%改善至-48%的模型平均偏差),但模型仍存在大幅低估。其他NMVOCs的变化相对较小。模拟的全球乙烷浓度的低偏差基本消除,解决了全球模拟中的一个长期问题。丙烷浓度有所改善,但仍被显著低估,这表明可能存在一个全球丙烷源缺失的情况。NMVOC排放物种组成的变化仅导致对流层O和OH浓度的微小变化。

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