气候变化领域集成服务门户(CCPortal): Secondary organic aerosol formation from smoldering and flaming combustion of biomass: A box model parametrization based on volatility basis set

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DOI	10.5194/acp-19-11461-2019
	Secondary organic aerosol formation from smoldering and flaming combustion of biomass: A box model parametrization based on volatility basis set
	Stefenelli G.; Jiang J.; Bertrand A.; Bruns E.A.; Pieber S.M.; Baltensperger U.; Marchand N.; Aksoyoglu S.; Prévôt A.S.H.; Slowik J.G.; El Haddad I.
发表日期	2019
ISSN	16807316
起始页码	11461
结束页码	11484
卷号	19 期号:17
英文摘要	Residential wood combustion remains one of the most important sources of primary organic aerosols (POA) and secondary organic aerosol (SOA) precursors during winter. The overwhelming majority of these precursors have not been traditionally considered in regional models, and only recently were lignin pyrolysis products and polycyclic aromatics identified as the principal SOA precursors from flaming wood combustion. The SOA yields of these components in the complex matrix of biomass smoke remain unknown and may not be inferred from smog chamber data based on single-compound systems. Here, we studied the ageing of emissions from flaming and smoldering-dominated wood fires in three different residential stoves, across a wide range of ageing temperatures ( - 10, 2 and 15 °C) and emission loads. Organic gases (OGs) acting as SOA precursors were monitored by a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), while the evolution of the aerosol properties during ageing in the smog chamber was monitored by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). We developed a novel box model based on the volatility basis set (VBS) to determine the volatility distributions of the oxidation products from different precursor classes found in the emissions, grouped according to their emission pathways and SOA production rates. We show for the first time that SOA yields in complex emissions are consistent with those reported in literature from single-compound systems. We identify the main SOA precursors in both flaming and smoldering wood combustion emissions at different temperatures. While single-ring and polycyclic aromatics are significant precursors in flaming emissions, furans generated from cellulose pyrolysis appear to be important for SOA production in the case of smoldering fires. This is especially the case at high loads and low temperatures, given the higher volatility of furan oxidation products predicted by the model. We show that the oxidation products of oxygenated aromatics from lignin pyrolysis are expected to dominate SOA formation, independent of the combustion or ageing conditions, and therefore can be used as promising markers to trace ageing of biomass smoke in the field. The model framework developed herein may be generalizable for other complex emission sources, allowing determination of the contributions of different precursor classes to SOA, at a level of complexity suitable for implementation in regional air quality models. © 2019 Author(s).
语种	英语
scopus关键词	aerosol composition; aerosol formation; biomass burning; combustion; oxidation; PAH; pyrolysis; qualitative analysis; winter
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/144158
作者单位	Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), Villigen, 5232, Switzerland; Aix Marseille Univ, CNRS, LCE, Marseille, France; Agence de l'Environnement et de la Maîtrise de l'Energie, 20 avenue du Gresillé, Angers Cedex 01, 49004, France; Empa, Laboratory for Air Pollution and Environmental Technology, Dübendorf, 8600, Switzerland; Washington State Department of Ecology, Lacey, WA, United States
推荐引用方式 GB/T 7714	Stefenelli G.,Jiang J.,Bertrand A.,et al. Secondary organic aerosol formation from smoldering and flaming combustion of biomass: A box model parametrization based on volatility basis set[J],2019,19(17).
APA	Stefenelli G..,Jiang J..,Bertrand A..,Bruns E.A..,Pieber S.M..,...&El Haddad I..(2019).Secondary organic aerosol formation from smoldering and flaming combustion of biomass: A box model parametrization based on volatility basis set.Atmospheric Chemistry and Physics,19(17).
MLA	Stefenelli G.,et al."Secondary organic aerosol formation from smoldering and flaming combustion of biomass: A box model parametrization based on volatility basis set".Atmospheric Chemistry and Physics 19.17(2019).