Radiocarbon‐derived source apportionment of fine carbonaceous aerosols before, during, and after the 2014 Asia‐Pacific Economic Cooperation (APEC) summit in Beijing, China

Liu, Junwen; Mo, Yangzhi; Li, Jun; Liu, Di; Shen, Chengde; Ding, Ping; Jiang, Haoyu; Cheng, Zhu; Zhang, Xiangyun; Tian, Chongguo; Chen, Yingjun; Zhang, Gan

doi:10.1002/2016jd024865

Cited by 18 publications

(12 citation statements)

References 64 publications

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“…In contrast, the results from the current study, using an extensive set of molecular 13 C/ 14 C data in China, strongly point to anthropogenic-fossil emissions as an important source of water-soluble OA. This is also supported by a large contribution of fossil sources to WSOC (30−60%) reported for both Chinese urban areas 52 – 55 and a receptor station in the southeast Yellow Sea intercepting a large regional footprint 11 , 12 . Taken together, these two sets of findings imply a significant missing pathway responsible for the enhancement in fossil fuel-derived water-soluble OA in China.…”

Section: Resultssupporting

confidence: 60%

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Zhang

Gustafsson

et al. 2022

Nat Commun

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Incomplete understanding of the sources of secondary organic aerosol (SOA) leads to large uncertainty in both air quality management and in climate change assessment. Chemical reactions occurring in the atmospheric aqueous phase represent an important source of SOA mass, yet, the effects of anthropogenic emissions on the aqueous SOA (aqSOA) are not well constrained. Here we use compound-specific dual-carbon isotopic fingerprints (δ13C and Δ14C) of dominant aqSOA molecules, such as oxalic acid, to track the precursor sources and formation mechanisms of aqSOA. Substantial stable carbon isotope fractionation of aqSOA molecules provides robust evidence for extensive aqueous-phase processing. Contrary to the paradigm that these aqSOA compounds are largely biogenic, radiocarbon-based source apportionments show that fossil precursors produced over one-half of the aqSOA molecules. Large fractions of fossil-derived aqSOA contribute substantially to the total water-soluble organic aerosol load and hence impact projections of both air quality and anthropogenic radiative forcing. Our findings reveal the importance of fossil emissions for aqSOA with effects on climate and air quality.

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Section: Resultssupporting

confidence: 60%

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Zhang

Gustafsson

et al. 2022

Nat Commun

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“…This is due to the fact that different approach we used for OC / EC separation, and sample selection in this study (selected two filter samples based on relatively lower and higher PM 2.5 concentration for each site) because of limitations for 14 C analysis (i.e., the bulk samples required and the high cost for 14 C measurement). However, the result is similar to those using the same approach (Liu et al, 2016b;Zong et al, 2016). A larger contribution of BB to EC was found in central and western China (i.e., Beijing, Lanzhou, Chengdu and Guiyang) (49 ∼ 63 %), where Guiyang had the largest proportion of BB in EC (63 ± 12 %), followed by Beijing (50 ± 2.0 %), Chengdu (50±1.8 %), Wuhan (48±10 %) and Nanjing (47±5 %); this shows that there are large amounts of BB emissions (e.g., from biofuel burning and outdoor fires) in western and central China during early winter.…”

Section: Radiocarbon Measurementssupporting

confidence: 67%

Sources of non-fossil-fuel emissions in carbonaceous aerosols during early winter in Chinese cities

Liu

Cheng

et al. 2017

Atmos. Chem. Phys.

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Abstract. China experiences frequent and severe haze outbreaks from the beginning of winter. Carbonaceous aerosols are regarded as an essential factor in controlling the formation and evolution of haze episodes. To elucidate the carbon sources of air pollution, source apportionment was conducted using radiocarbon ( 14 C) and unique molecular organic tracers. Daily 24 h PM 2.5 samples were collected continuously from October 2013 to November 2013 in 10 Chinese cities. The 14 C results indicated that non-fossil-fuel (NF) emissions were predominant in total carbon (TC; average = 65 ± 7 %). Approximately half of the EC was derived primarily from biomass burning (BB) (average = 46±11 %), while over half of the organic carbon (OC) fraction comprised NF (average = 68 ± 7 %). On average, the largest contributor to TC was NF-derived secondary OC (SOC nf ), which accounted for 46 ± 7 % of TC, followed by SOC derived from fossil fuels (FF) (SOC f ; 16 ± 3 %), BB-derived primary OC (POC bb ; 13 ± 5 %), POC derived from FF (POC f ; 12 ± 3 %), EC derived from FF (EC f ; 7±2 %) and EC derived from BB (EC bb ; 6 ± 2 %). The regional background carbonaceous aerosol composition was characterized by NF sources; POCs played a major role in northern China, while SOCs contributed more in other regions. However, during haze episodes, there were no dramatic changes in the carbon source or composition in the cities under study, but the contribution of POC from both FF and NF increased significantly.

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“…In addition, LG concentrations at the rural site were higher than those at the urban site in both winter and summer. This pattern is consistent with previous measurements in Table 3 (Chen et al, 2018;Kang et al, 2018;Li et al, 2018;Liu et al, 2016b;Salma et al, 2017;Sullivan et al, 2019;Yan et al, 2019;Zhu et al, 2017). The Pearson correlations of LG with PM 2.5 , OC, and EC at IAP and PG are shown in Table S1.…”

Section: Biomass Burningsupporting

confidence: 91%

Source apportionment of carbonaceous aerosols in Beijing with radiocarbon and organic tracers: insight into the differences between urban and rural sites

Hou

Liu

et al. 2021

Atmos. Chem. Phys.

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Abstract. Carbonaceous aerosol is a dominant component of fine particles in Beijing. However, it is challenging to apportion its sources. Here, we applied a newly developed method which combined radiocarbon (14C) with organic tracers to apportion the sources of fine carbonaceous particles at an urban (IAP) and a rural (PG) site of Beijing. PM2.5 filter samples (24 h) were collected at both sites from 10 November to 11 December 2016 and from 22 May to 24 June 2017. 14C was determined in 25 aerosol samples (13 at IAP and 12 at PG) representing low pollution to haze conditions. Biomass burning tracers (levoglucosan, mannosan, and galactosan) in the samples were also determined using gas chromatography–mass spectrometry (GC-MS). Higher contributions of fossil-derived OC (OCf) were found at the urban site. The OCf / OC ratio decreased in the summer samples (IAP: 67.8 ± 4.0 % in winter and 54.2 ± 11.7 % in summer; PG: 59.3 ± 5.7 % in winter and 50.0 ± 9.0 % in summer) due to less consumption of coal in the warm season. A novel extended Gelencsér (EG) method incorporating the 14C and organic tracer data was developed to estimate the fossil and non-fossil sources of primary and secondary OC (POC and SOC). It showed that fossil-derived POC was the largest contributor to OC (35.8 ± 10.5 % and 34.1 ± 8.7 % in wintertime for IAP and PG, 28.9 ± 7.4 % and 29.1 ± 9.4 % in summer), regardless of season. SOC contributed 50.0 ± 12.3 % and 47.2 ± 15.5 % at IAP and 42.0 ± 11.7 % and 43.0 ± 13.4 % at PG in the winter and summer sampling periods, respectively, within which the fossil-derived SOC was predominant and contributed more in winter. The non-fossil fractions of SOC increased in summer due to a larger biogenic component. Concentrations of biomass burning OC (OCbb) are resolved by the extended Gelencsér method, with average contributions (to total OC) of 10.6 ± 1.7 % and 10.4 ± 1.5 % in winter at IAP and PG and 6.5 ± 5.2 % and 17.9 ± 3.5 % in summer, respectively. Correlations of water-insoluble OC (WINSOC) and water-soluble OC (WSOC) with POC and SOC showed that although WINSOC was the major contributor to POC, a non-negligible fraction of WINSOC was found in SOC for both fossil and non-fossil sources, especially during winter. In summer, a greater proportion of WSOC from non-fossil sources was found in SOC. Comparisons of the source apportionment results with those obtained from a chemical mass balance model were generally good, except for the cooking aerosol.

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Radiocarbon‐derived source apportionment of fine carbonaceous aerosols before, during, and after the 2014 Asia‐Pacific Economic Cooperation (APEC) summit in Beijing, China

Cited by 18 publications

References 64 publications

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China

Sources of non-fossil-fuel emissions in carbonaceous aerosols during early winter in Chinese cities

Source apportionment of carbonaceous aerosols in Beijing with radiocarbon and organic tracers: insight into the differences between urban and rural sites

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