High contributions of fossil sources to more volatile organic aerosol

Ni, Haiyan; Huang, Ru‐Jin; Cao, Junji; Dai, Wenting; Zhou, Jiaqi; Deng, Haoyue; Aerts-Bijma, Anita; Meijer, H. A. J.; Dusek, Ulrike

doi:10.5194/acp-19-10405-2019

Cited by 12 publications

(10 citation statements)

References 97 publications

(120 reference statements)

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“…The presented overall average ffossil(OC) for winter 2016/2017 in Beijing (66 ± 3%) was higher than that in Xi'an (46 ± 3%), consistent with previously reported ffossil(OC) in Beijing and Xi'an (Zhang et al, 2015;Ni et al, 2019a). Lower ffossil(OC) values in winter were reported for Chongqing (24%), and higher ffossil(OC) was observed in Taiyuan (71%) during winter 2013/2014 (Ni et al, 2019a). The comparison of ffossil(EC) and ffossil(OC) in different Chinese cities indicates that the relative importance of fossil sources in carbonaceous aerosols vary spatially, and can change over the years.…”

Section: Fossil and Non-fossil Contributions To Ec And Ocsupporting

confidence: 88%

“…Radiocarbon ( 14 C) analysis of carbonaceous aerosols is the most direct and effective method to distinguish their main sources, exploiting the fact that OC and EC of fossil origins (i.e., vehicle emissions, coal combustion) do not contain 14 C (Heal, 2014;Cao et al, 2017). 14 C analysis of OC and EC separately provide a clear-cut division of carbonaceous aerosols into four major fractions: fossil OC, non-fossil OC (e.g., OC from biomass burning, biogenic emissions and cooking), fossil EC and biomassburning EC (e.g., Gustafsson et al, 2009;Szidat et al, 2009;Zotter et al, 2014;Dusek et al, 2017;Ni et al, 2018Ni et al, , 2019a.…”

Section: Introductionmentioning

confidence: 99%

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Measurement report: Dual-carbon isotopic characterization of carbonaceous aerosol in Beijing and Xi'an: distinctions in primary versus secondary sources

Huang

Cosijn

et al. 2020

Preprint

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Abstract. To mitigate haze pollution in China, a better understanding of the sources of carbonaceous aerosols is required due to the complexity in multiple emissions and atmospheric processes. Here we combined the analysis of radiocarbon and the stable isotope 13C to investigate the sources and formation of carbonaceous aerosols collected in two Chinese megacities (Beijing and Xi’an) during severe haze events of “red alarm” level from December 2016 to January 2017. In Xi’an, liquid fossil fuel combustion was the dominant source of elemental carbon (EC; 44 %–57 %), followed by biomass burning (25 %–29 %) and coal combustion (17 %–29 %). In Beijing, coal combustion contributed 45%–61% of EC and biomass burning (17 %–24 %) and liquid fossil fuel combustion (22 %–33 %) contributed less. Non-fossil sources contributed 51 %–56 % of organic carbon (OC) in Xi’an and fossil sources contributed 63 %–69 % of OC in Beijing. Secondary OC (SOC) was largely contributed by non-fossil sources in Xi’an (56 ± 6 %) and by fossil sources in Beijing (75 ± 10 %), especially during haze periods. The fossil vs. non-fossil contributions to OC and EC did not change drastically during haze events in both Xi’an and Beijing. However, compared to clean periods, the contribution of coal combustion to EC during haze periods increased in Xi’an and decreased in Beijing. During clean periods, primary OC from biomass burning and fossil sources constituted ~ 70 % of OC in Xi’an and ~ 53 % of OC in Beijing. From clean to haze periods, the contribution of SOC to total OC increased in Xi’an, but decreased in Beijing, suggesting that contribution of secondary organic aerosol formation to increased OC during haze periods was more efficient in Xi’an than in Beijing. In Beijing, the high SOC fraction in total OC during clean periods was mainly due to elevated contribution from non-fossil SOC. In Xi’an, a slight day-night difference was observed during clean period, with enhanced fossil contributions to OC and EC during the day. This day-night difference was negligible during severe haze periods, likely due to enhanced accumulation of pollutants under stagnant weather conditions.

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Section: Fossil and Non-fossil Contributions To Ec And Ocsupporting

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Measurement report: Dual-carbon isotopic characterization of carbonaceous aerosol in Beijing and Xi'an: distinctions in primary versus secondary sources

Huang

Cosijn

et al. 2020

Preprint

Self Cite

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“…The results imply the importance of nonfossil OA formation from biogenic and/or biomass burning influences in different seasons even in a city with high traffic emissions mainly based on fossil fuel combustion (LUBW, 2019). This is similar to previous studies in other European cities such as Barcelona, Spain (Mohr et al, 2012), and some megacities in China (Ni et al, 2019). In the next section, we investigate the volatility of OOA compounds measured by CIMS, which can influence their lifetime in the atmosphere and thus air quality.…”

Section: Molecular Composition Of Ooasupporting

confidence: 75%

Seasonal characteristics of organic aerosol chemical composition and volatility in Stuttgart, Germany

et al. 2019

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Abstract. The chemical composition and volatility of organic aerosol (OA) particles were investigated during July–August 2017 and February–March 2018 in the city of Stuttgart, one of the most polluted cities in Germany. Total non-refractory particle mass was measured with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS; hereafter AMS). Aerosol particles were collected on filters and analyzed in the laboratory with a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO-HR-ToF-CIMS; hereafter CIMS), yielding the molecular composition of oxygenated OA (OOA) compounds. While the average organic mass loadings are lower in the summer period (5.1±3.2 µg m−3) than in the winter period (8.4±5.6 µg m−3), we find relatively larger mass contributions of organics measured by AMS in summer (68.8±13.4 %) compared to winter (34.8±9.5 %). CIMS mass spectra show OOA compounds in summer have O : C of 0.82±0.02 and are more influenced by biogenic emissions, while OOA compounds in winter have O : C of 0.89±0.06 and are more influenced by biomass burning emissions. Volatility parametrization analysis shows that OOA in winter is less volatile with higher contributions of low-volatility organic compounds (LVOCs) and extremely low-volatility organic compounds (ELVOCs). We partially explain this by the higher contributions of compounds with shorter carbon chain lengths and a higher number of oxygen atoms, i.e., higher O : C in winter. Organic compounds desorbing from the particles deposited on the filter samples also exhibit a shift of signal to higher desorption temperatures (i.e., lower apparent volatility) in winter. This is consistent with the relatively higher O : C in winter but may also be related to higher particle viscosity due to the higher contributions of larger-molecular-weight LVOCs and ELVOCs, interactions between different species and/or particles (particle matrix), and/or thermal decomposition of larger molecules. The results suggest that whereas lower temperature in winter may lead to increased partitioning of semi-volatile organic compounds (SVOCs) into the particle phase, this does not result in a higher overall volatility of OOA in winter and that the difference in sources and/or chemistry between the seasons plays a more important role. Our study provides insights into the seasonal variation of the molecular composition and volatility of ambient OA particles and into their potential sources.

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“…Radiocarbon ( 14 C) analysis of carbonaceous aerosols is the most direct and effective method to distinguish their main sources, exploiting the fact that OC and EC of fossil origins (i.e., vehicle emissions, coal combustion) do not contain 14 C (Heal, 2014;Cao et al, 2017;Dusek et al, 2013). The 14 C analysis of OC and EC separately provides a clear-cut division of carbonaceous aerosols into four major fractions: fossil OC, non-fossil OC (e.g., OC from biomass burning, biogenic emissions, and cooking), fossil EC and biomass-burning EC (e.g., Gustafsson et al, 2009;Zotter et al, 2014;Dusek et al, 2017;Ni et al, 2018Ni et al, , 2019a. For example, Liu et al (2014) demonstrated that fossil sources including coal burning and vehicle emissions dominated EC during winter haze events in Guangzhou, China.…”

Section: Introductionmentioning

confidence: 99%

Measurement report: dual-carbon isotopic characterization of carbonaceous aerosol reveals different primary and secondary sources in Beijing and Xi'an during severe haze events

Huang

Cosijn

et al. 2020

Atmos. Chem. Phys.

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Abstract. To mitigate haze pollution in China, a better understanding of the sources of carbonaceous aerosols is required due to the complexity in multiple emissions and atmospheric processes. Here we combined the analysis of radiocarbon and the stable isotope 13C to investigate the sources and formation of carbonaceous aerosols collected in two Chinese megacities (Beijing and Xi'an) during severe haze events of a “red alarm” level from December 2016 to January 2017. The haze periods with daily PM2.5 concentrations as high as ∼ 400 µg m−3 were compared to subsequent clean periods (i.e., PM2.5 less than median concentrations during the winter 2016/2017) with PM2.5 concentrations below 100 µg m−3 in Xi'an and below 20 µg m−3 in Beijing. In Xi'an, liquid fossil fuel combustion was the dominant source of elemental carbon (EC; 44 %–57 %), followed by biomass burning (25 %–29 %) and coal combustion (17 %–29 %). In Beijing, coal combustion contributed 45 %–61 % of EC, and biomass burning (17 %–24 %) and liquid fossil fuel combustion (22 %–33 %) contributed less. Non-fossil sources contributed 51 %–56 % of organic carbon (OC) in Xi'an, and fossil sources contributed 63 %–69 % of OC in Beijing. Secondary OC (SOC) was largely contributed by non-fossil sources in Xi'an (56±6 %) and by fossil sources in Beijing (75±10 %), especially during haze periods. The fossil vs. non-fossil contributions to OC and EC did not change drastically during haze events in both Xi'an and Beijing. However, compared to clean periods, the contribution of coal combustion to EC during haze periods increased in Xi'an and decreased in Beijing. During clean periods, primary OC from biomass burning and fossil sources constituted ∼ 70 % of OC in Xi'an and ∼ 53 % of OC in Beijing. From clean to haze periods, the contribution of SOC to total OC increased in Xi'an but decreased in Beijing, suggesting that the contribution of secondary organic aerosol formation to increased OC during haze periods was more efficient in Xi'an than in Beijing. In Beijing, the high SOC fraction in total OC during clean periods was mainly due to an elevated contribution from non-fossil SOC. In Xi'an, a slight day–night difference was observed during the clean period with enhanced fossil contributions to OC and EC during the day. This day–night difference was negligible during severe haze periods, likely due to the enhanced accumulation of pollutants under stagnant weather conditions.

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High contributions of fossil sources to more volatile organic aerosol

Cited by 12 publications

References 97 publications

Measurement report: Dual-carbon isotopic characterization of carbonaceous aerosol in Beijing and Xi'an: distinctions in primary versus secondary sources

Measurement report: Dual-carbon isotopic characterization of carbonaceous aerosol in Beijing and Xi'an: distinctions in primary versus secondary sources

Seasonal characteristics of organic aerosol chemical composition and volatility in Stuttgart, Germany

Measurement report: dual-carbon isotopic characterization of carbonaceous aerosol reveals different primary and secondary sources in Beijing and Xi'an during severe haze events

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