2020年夏季法国巴黎地区有机气体和颗粒化合物的源解析

IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES
Leïla Simon , Olivier Favez , Jean-Eudes Petit , Francesco Canonaco , Jay G. Slowik , Caroline Marchand , Valérie Gros
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引用次数: 0

摘要

气态和颗粒有机化合物是大气化学的关键组成部分,更好地了解它们的组成、来源和过程对于限制它们的影响至关重要。使用正矩阵分解(PMF)的源分配通常用于此类研究。将有机气溶胶数据与其气态前体相结合被证明是一种很有前途的方法,但迄今为止很少有人尝试使用PMF来改进它们的起源。在这项研究中,在位于巴黎地区郊区的SIRTA站进行了同步连续质子转移反应质谱仪(PTR-MS)和气溶胶化学形态监测仪(ACSM)测量。然后,在夏季(2020年6月至8月)使用这两种仪器的组合数据集进行探索性PMF分析,以调查有机化合物的来源和过程,特别是生物源排放和重要光化学反应对一年中这一时期二次有机气溶胶(SOA)形成的影响。需要具体的参数和评价程序来确保这两种工具在PMF模型中的等效表示。在模型化残差分析的基础上,对PTR-MS不确定度进行了控制和优化。得到了7个主要因素,分别是人为来源(类碳氢化合物有机物、类烹饪有机物)、主要生物源挥发性有机物、夜间VOC、氧化有机物、老化有机物和一个特定的异戊二烯氧化因子,该因子对VOC和OA分别贡献11%和4%。与单仪器PMFs相比,获得了更多的因素,特别是包括通常仅使用ACSM数据无法解决的类似烹饪的因素。该方法还显示了PTR-MS变量的更好的数学性能(组合PMF的平均绝对缩放残差(11.2)低于仅PTR-MS的PMF(38.2)),并且在组合PMF中ACSM变量的因素分离效果更好。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Source apportionment of organic gaseous and particulate compounds using a combined positive matrix factorization approach in summer (2020) in the Paris region (France)
Gaseous and particulate organic compounds are key components of atmospheric chemistry and better understanding their composition, sources and processes is essential to limit their impacts. Source apportionment using positive matrix factorization (PMF) is customarily performed for such studies. Combining organic aerosol data with their gaseous precursors was shown to be a promising approach, however very rarely attempted so far, to refine their origins using PMF. In this study, co-located continuous proton-transfer-reaction mass spectrometer (PTR-MS) and aerosol chemical speciation monitor (ACSM) measurements were performed at the suburban SIRTA station located in the Paris region. A combined dataset using both instruments during summer (June–August 2020) was then used in an exploratory PMF analysis to investigate the sources and processes of organic compounds, particularly the influences of biogenic emissions and important photochemical reactions on the formation of secondary organic aerosol (SOA) in this period of the year. Specific parameters and evaluation procedures were needed to ensure an equivalent representation of both instruments in the PMF model. A weighing factor was applied to the PTR-MS uncertainties which was controlled and optimized based on the analysis of the modelled scaled residuals. Seven main factors were obtained, describing anthropogenic sources (hydrocarbon-like organics, cooking-like organics), primary biogenic volatile organics, nighttime VOC, oxidized organics, aged organics and a specific isoprene oxidation factor which contributed 11 % to VOC and 4 % to OA. Compared to single-instrument PMFs, more factors were obtained, notably including the cooking-like factor which is not usually resolved using only ACSM data. This method also showed a better mathematical performance for the PTR-MS variables (mean absolute scaled residuals lower for the combined PMF (11.2) than for the PTR-MS-only PMF (38.2)) and a better separation of the factors for the ACSM variables in the combined PMF.
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来源期刊
Atmospheric Environment
Atmospheric Environment 环境科学-环境科学
CiteScore
9.40
自引率
8.00%
发文量
458
审稿时长
53 days
期刊介绍: Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.
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