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DOI | 10.5194/acp-18-2199-2018 |
Bulk and molecular-level characterization of laboratory-aged biomass burning organic aerosol from oak leaf and heartwood fuels | |
Fortenberry, Claire F.1; Walker, Michael J.1; Zhang, Yaping1; Mitroo, Dhruv1,3; Brune, William H.2; Williams, Brent J.1 | |
2018-02-15 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:3页码:2199-2224 |
文章类型 | Article |
语种 | 英语 |
国家 | USA |
英文摘要 | The chemical complexity of biomass burning organic aerosol (BBOA) greatly increases with photochemical aging in the atmosphere, necessitating controlled laboratory studies to inform field observations. In these experiments, BBOA from American white oak (Quercus alba) leaf and heartwood samples was generated in a custom-built emissions and combustion chamber and photochemically aged in a potential aerosol mass (PAM) flow reactor. A thermal desorption aerosol gas chromatograph (TAG) was used in parallel with a high-resolution time-of-flight aerosol mass spectrometer (AMS) to analyze BBOA chemical composition at different levels of photochemical aging. Individual compounds were identified and integrated to obtain relative decay rates for key molecules. A recently developed chromatogram binning positive matrix factorization (PMF) technique was used to obtain mass spectral profiles for factors in TAG BBOA chromatograms, improving analysis efficiency and providing a more complete determination of unresolved complex mixture (UCM) components. Additionally, the recently characterized TAG decomposition window was used to track molecular fragments created by the decomposition of thermally labile BBOA during sample desorption. We demonstrate that although most primary (freshly emitted) BBOA compounds deplete with photochemical aging, certain components eluting within the TAG thermal decomposition window are instead enhanced. Specifically, the increasing trend in the decomposition m/z 44 signal (CO2+) indicates formation of secondary organic aerosol (SOA) in the PAM reactor. Sources of m/z 60 (C2H4O2+), typically attributed to freshly emitted BBOA in AMS field measurements , were also investigated. From the TAG chemical speciation and decomposition window data, we observed a decrease in m/z 60 with photochemical aging due to the decay of anhydrosugars (including levoglucosan) and other compounds , as well as an increase in m/z 60 due to the formation of thermally labile organic acids within the PAM reactor, which decompose during TAG sample desorption. When aging both types of BBOA (leaf and heartwood), the AMS data exhibit a combination of these two contributing effects, causing limited change to the overall m/z 60 signal. Our observations demonstrate the importance of chemically speciated data in fully understanding bulk aerosol measurements provided by the AMS in both laboratory and field studies. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000425311300001 |
WOS关键词 | RESIDENTIAL WOOD COMBUSTION ; OXIDATION FLOW REACTORS ; GAS-CHROMATOGRAPH TAG ; THERMAL-DESORPTION ; BROWN CARBON ; HETEROGENEOUS OXIDATION ; ATMOSPHERIC PARTICLES ; HOURLY MEASUREMENTS ; MASS-SPECTROMETER ; RADICAL CHEMISTRY |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/18387 |
专题 | 地球科学 |
作者单位 | 1.Washington Univ, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA; 2.Penn State Univ, Dept Meteorol & Atmospher Sci, State Coll, PA 16801 USA; 3.Univ Miami, Rosenstiel Sch Marine & Atmospher Sci, Dept Atmospher Sci, Miami, FL 33149 USA |
推荐引用方式 GB/T 7714 | Fortenberry, Claire F.,Walker, Michael J.,Zhang, Yaping,et al. Bulk and molecular-level characterization of laboratory-aged biomass burning organic aerosol from oak leaf and heartwood fuels[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(3):2199-2224. |
APA | Fortenberry, Claire F.,Walker, Michael J.,Zhang, Yaping,Mitroo, Dhruv,Brune, William H.,&Williams, Brent J..(2018).Bulk and molecular-level characterization of laboratory-aged biomass burning organic aerosol from oak leaf and heartwood fuels.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(3),2199-2224. |
MLA | Fortenberry, Claire F.,et al."Bulk and molecular-level characterization of laboratory-aged biomass burning organic aerosol from oak leaf and heartwood fuels".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.3(2018):2199-2224. |
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