Quantifying Atmospheric Parameter Ranges for Ambient Secondary Organic Aerosol Formation

Quantifying Atmospheric Parameter Ranges for Ambient Secondary Organic Aerosol Formation
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量化环境二次有机气溶胶形成的大气参数范围

DOI:
10.1021/acsearthspacechem.1c00090
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发表时间:
2021
影响因子:
3.4
通讯作者:
Barsanti, Kelley C.
Barsanti, Kelley C.
中科院分区:
化学3区
文献类型:
--
作者:
Porter, William C.;Jimenez, Jose L.;Barsanti, Kelley C.

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在过去的几十年里,人们对大气中二次有机气溶胶(SOA)形成和演化的基本化学和物理过程的认识迅速发展。其中许多进步是通过实验室研究实现的,特别是在环境室中进行的SOA研究。这些研究的结果被用来开发简化表示SOA的形成在区域和全球尺度的空气质量模型。虽然它是已知的,在何种程度上,实验室实验可以代表周围的大气有限制,一直没有系统的调查,什么定义的SOA形成的背景下的大气相关性。在这项工作中,GEOS-Chem 12.3版被用来定量描述大气相关的化学和气象参数范围,这些参数对于预测SOA的质量、组成和物理特性至关重要。就某些参数而言,与大气有关的范围一般在实验室研究中得到充分体现。然而,对于其他参数,大气相关范围与典型实验室条件之间存在重大差距。例如,寒冷的冬季(低于0 °C)和潮湿(大于70%RH)条件在地球表面相对常见,但在已公布的室数据中表现不佳。此外,相对湿度和有机气溶胶质量的重叠室研究和环境条件之间几乎不存在。对于存在显著差距的参数,需要进行扩展的实验室研究和/或建立机理模型,以弥补这些差距。
Understanding of the fundamental chemical and physical processes that lead to the formation and evolution of secondary organic aerosol (SOA) in the atmosphere has been rapidly advancing over the past decades. Many of these advancements have been achieved through laboratory studies, particularly SOA studies conducted in environmental chambers. Results from such studies are used to develop simplified representations of SOA formation in regional- and global-scale air quality models. Although it is known that there are limitations in the extent to which laboratory experiments can represent the ambient atmosphere, there have been no systematic surveys of what defines atmospheric relevance in the context of SOA formation. In this work, GEOS-Chem version 12.3 was used to quantitatively describe atmospherically relevant ranges of chemical and meteorological parameters critical for predictions of the mass, composition, and physical properties of SOA. For some parameters, atmospherically relevant ranges are generally well represented in laboratory studies. However for other parameters, significant gaps exist between atmospherically relevant ranges and typical laboratory conditions. For example, cold winter (less than 0 °C) and humid (greater than 70% RH) conditions are relatively common on the Earth’s surface but are poorly represented in published chamber data. Furthermore, the overlap in relative humidity and organic aerosol mass between chamber studies and ambient conditions is almost nonexistent. For parameters with significant gaps, extended laboratory studies and/or mechanistic models are needed to bridge these gaps.
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