Mass spectral characterization of primary emissions and implications in source apportionment of organic aerosol

Xu, Weiqi; He, Yuehui; Qiu, Yanmei; Chen, Chun; Xie, Conghui; Lu, Ling; Li, Zhijie; Sun, Jiaxing; Li, Junyao; Fu, Pingqing; Wang, Zifa; Worsnop, Douglas R.; Sun, Yele

doi:10.5194/amt-13-3205-2020

Cited by 39 publications

(45 citation statements)

References 68 publications

(96 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The four Chinese dishes had prominent peaks at m/z 41, m/z 43 and m/z 55 (generated from C3H5 + and C3H7 + , C4H7 + ) which was qualitatively consistent with mass spectra of primary COA in other studies (Xu et al, 2020). As described by He et al (2010), the most abundant ion fragments at m/z 41 and m/z 55 from primary Chinese cooking emissions are resulting from unsaturated fatty acids (He et al, 2010).…”

Section: Resultssupporting

confidence: 85%

“…However, based on collocated AMS measurements and factor analysis results, the SOA formed by vehicle and cooking sources cannot be effectively resolved from the total SOA due to the lack of secondary mass spectral profiles. The POA mass spectral profiles based on AMS including HOA (Collier et al, 2015), BBOA (Alfarra et al, 2007;He et al, 2010;Xu et al, 2020), and COA (He et al, 2010;Liu et al, 2017;Mohr et al, 2012;Xu et al, 2020) have been fully explored in laboratory studies, and applied as constraint factors into the ME-2 model in the ambient air. Some studies have made it possible to quantify biogenic secondary aerosol products of a single precursor, such as isoprene oxidation products (IEPOX) (Budisulistiorini et al, 2013;Hu et al, 2016b), and have been extended to the urban atmosphere to obtain an IEPOX-SOA factor via PMF analysis of OA spectra (Zhang et al, 2017b).…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Mass spectral characterization of secondary organic aerosol from urban lifestyle sources emissions

Zhu

Guo

et al. 2021

Preprint

View full text Add to dashboard Cite

Abstract. In the present work, we conducted experiments of secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicle) to characterize the mass spectral features of primary organic aerosol (POA) and SOA using an high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Our results showed that the cooking styles have greater impact on aged COA mass spectra than oxidation condition. However, the oxidation conditions affect the aged HOA spectra more significantly than vehicle operation conditions. In our study, we use mass spectra similarity analysis and positive matrix factorization (PMF) analysis to establish the POA and SOA mass spectra of these two typical lifestyle sources. These mass spectra are used as source constraints in a multilinear engine (ME-2) model to apportion the OA sources in the atmosphere. Comparing with the traditional ambient PMF results, the improved ME-2 model can better quantify the contribution of POA and SOA from life-style sources. Our work, for the first time, establishes the vehicle and cooking SOA source profiles, and can be further used in the OA source apportionment in the ambient atmosphere.

show abstract

Section: Resultssupporting

confidence: 85%

Section: Introductionmentioning

confidence: 99%

Mass spectral characterization of secondary organic aerosol from urban lifestyle sources emissions

Zhu

Guo

et al. 2021

Preprint

View full text Add to dashboard Cite

show abstract

“…x in mass spectra of SOA in winter in Beijing. The OA factors representing different sources were identified by PMF, and detailed PMF analyses from the three campaigns have been given in Xu et al (2021) and Chen et al (2021).…”

Section: Discussionmentioning

confidence: 99%

Estimation of particulate organic nitrates from thermodenuder–aerosol mass spectrometer measurements in the North China Plain

Takeuchi

Chen

et al. 2021

Atmos. Meas. Tech.

Self Cite

View full text Add to dashboard Cite

Abstract. Particulate organic nitrates (pON) are an important component of secondary organic aerosol in biogenic-emission-dominant environments and play a critical role in NOx cycles. However, estimation of pON has been a challenge in polluted environments, e.g., North China Plain, with high concentrations of inorganic nitrate and NOx. Here we developed a method for estimation of pON from the measurements of high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally correlated well with those estimated from positive matrix factorization of combined organic and inorganic mass spectra and from the ratio of NO+ to NO2+ (NOx+ ratio), yet they had improvements in reducing negative values due to the influences of high concentration of inorganic nitrate and constant NOx+ ratio of organic nitrates (RON). By applying this approach to the measurements at an urban (Beijing) and a rural site (Gucheng) in summer and winter in the North China Plain, we estimated that the average mass concentrations of NO3,org (1.8 µg m−3 vs. 1.0 µg m−3) and pON to OA (27.5 % vs. 14.8 %) were higher in summer than in winter in Beijing, indicating more pON formation in biogenically and anthropogenically mixed environments. In addition, the average NO3,org loading in Gucheng was 1.9 µg m−3, and the pON at the rural site also showed higher contribution to OA than that in Beijing during wintertime due to higher primary emissions and gaseous precursors in Gucheng. In addition, RON was determined and showed considerable differences between day–night and clean–polluted periods, highlighting the complexity of pON compounds from different chemical pathways (e.g., OH and NO3 oxidation) and sources.

show abstract

“…The NO x + signals assigned to POA in winter in Beijing were much higher than those in source emission experiments. For example, f NO+ (3.5%) and f NO2+ (1.5%, fractions of NO + or NO 2 + in total mass spectrum) of biomass burning OA in winter in Beijing (Fig.S3) were higher than that from burning of different biofuels (f NO+ =0.9% and f NO2+ =0.65%) (Xu et al, 2020). Further analysis suggested that the episodes dominated by POA also resulted in higher pON loadings from the "PMF method" in winter in Beijing.…”

Section: Intercomparisonsmentioning

confidence: 97%

“…However, the separation of inorganic and organic NO x + may be limited by the bilinear model depending on the correlations between inorganic nitrate and pON. In addition, some primary organic aerosol (POA) factors from "PMF method" also contained much higher NO + or NO 2 + compared to directly measured mass spectrum of primary emissions (Xu et al, 2020) (Fig. S1), increasing the uncertainties in quantification of pON.…”

Section: Introductionmentioning

confidence: 99%

Estimation of particulate organic nitrates from thermodenuder-aerosol mass spectrometer measurements in North China Plain

Xu¹,

Takeuchi²,

Chen³

et al. 2020

Preprint

Self Cite

View full text Add to dashboard Cite

Abstract. Particulate organic nitrates (pON) are an important component of secondary organic aerosol in biogenic emission dominant environments, and play a critical role in NOx cycles. However, estimation of pON has been a challenge in polluted environments, e.g., North China Plain with high concentrations of inorganic nitrate and NOx. Here we developed a method for estimation of pON from the measurements of high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally correlated well with those estimated from positive matrix factorization of combined organic and inorganic mass spectra and from the ratio of NO+ to NO2+ (NOx+ ratio), yet had improvements in reducing negative values due to the influences of high concentration of inorganic nitrate and constant NOx+ ratio of organic nitrates (RON). By applying this approach to the measurements at an urban (Beijing) and a rural site (Gucheng) in summer and winter in North China Plain, we estimated that the average mass concentrations of NO3,org (1.8 µg m−3 vs.1.0 µg m−3) and pON to OA (27.5 % vs. 14.8 %) were higher in summer than in winter in Beijing, indicating more pON formation in biogenically and anthropogenically mixed environments. In addition, the average NO3,org loading in Gucheng was 1.9 µg m−3, and the pON at the rural site also showed higher contribution to OA than that in Beijing during wintertime due to higher primary emissions and gaseous precursors in Gucheng. In addition, RON was determined and showed considerable differences between day-night and clean-polluted periods, highlighting the complexity of pON compounds from different chemical pathways (e.g., OH and NO3 oxidation) and sources.

show abstract

Mass spectral characterization of primary emissions and implications in source apportionment of organic aerosol

Cited by 39 publications

References 68 publications

Mass spectral characterization of secondary organic aerosol from urban lifestyle sources emissions

Mass spectral characterization of secondary organic aerosol from urban lifestyle sources emissions

Estimation of particulate organic nitrates from thermodenuder–aerosol mass spectrometer measurements in the North China Plain

Estimation of particulate organic nitrates from thermodenuder-aerosol mass spectrometer measurements in North China Plain

Contact Info

Product

Resources

About