Source apportionment of elevated wintertime PAHs by compound-specific radiocarbon analysis

Sheesley, Rebecca J.; Kruså, Martin; Krecl, Patricia; Johansson, Christer; Gustafsson, Örjan

doi:10.5194/acp-9-3347-2009

Cited by 46 publications

(34 citation statements)

References 51 publications

(77 reference statements)

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“…[24] The soot-BC d 13 C values varied between À27.8 and À17.0‰ (À23.1 À24.5 À22.3 ‰; Table S1 in the auxiliary material). 1 Overall, these heterogeneous isotopic signatures are in the range of that of other combustion products (e.g., PAHs) in aerosols (À29 to À21‰ [Norman et al, 1999;Okuda et al, 2002;Mandalakis et al, 2004;Sheesley et al, 2009]). However, source apportionment based on soot-BC d 13 C values is difficult due to (i) overlapping d 13 C-BC signatures of different combustion sources; (ii) the variability of the d 13 C values depending on both the isotopic signature of the parent fuels [O'Malley et al, 1997;McRae et al, 1999] and the combustion temperature [McRae et al, 1999]; and (iii) the possibility of fractionation during incomplete combustion.…”

Section: Concentration and Sources Of Soot Black Carbon In The Swedismentioning

confidence: 99%

The sequestration sink of soot black carbon in the Northern European Shelf sediments

Sánchez-García¹,

Cato²,

Gustafsson³

2012

Global Biogeochemical Cycles

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To test the hypothesis that ocean margin sediments are a key final repository in the large‐scale biogeospheric cycling of soot black carbon (soot‐BC), an extensive survey was conducted along the ∼2,000 km stretch of the Swedish Continental Shelf (SCS). The soot‐BC content in the 120 spatially distributed SCS sediments was 0.180.130.26% dw (median with interquartile ranges), corresponding to ∼5% of total organic carbon. Using side‐scan sonar constraints to estimate the areal fraction of postglacial clay sediments that are accumulation bottoms (15% of SCS), the soot‐BC inventory in the SCS mixed surface sediment was estimated at ∼4,000 Gg. Combining this with radiochronological constraints on sediment mass accumulation fluxes, the soot‐BC sink on the SCS was ∼300 Gg/yr, which yielded an area‐extrapolated estimate for the Northern European Shelf (NES) of ∼1,100 Gg/yr. This sediment soot‐BC sink is ∼50 times larger than the river discharge fluxes of soot‐BC to these coastal waters, however, of similar magnitude as estimates of atmospheric soot‐BC emission from the upwind European continent. While large uncertainties remain regarding the large‐scale to global BC cycle, this study combines with two previous investigations to suggest that continental shelf sediments are a major final repository of atmospheric soot‐BC. Future progress on the soot‐BC cycle and how it interacts with the full carbon cycle is likely to benefit from14C determinations of the sedimentary soot‐BC and similar extensive studies of coastal sediment in complementary regimes such as off heavily soot‐BC‐producing areas in S and E Asia and on the large pan‐Arctic shelf.

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Section: Concentration and Sources Of Soot Black Carbon In The Swedismentioning

confidence: 99%

The sequestration sink of soot black carbon in the Northern European Shelf sediments

Sánchez-García¹,

Cato²,

Gustafsson³

2012

Global Biogeochemical Cycles

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“…Sheesley et al [79] Table 2: A summary of studies reporting the fraction non-fossil carbon in atmospheric PM published since the mid-2000s. The focus is on data relating to the fraction non-fossil carbon in PM total carbon (TC) but data for non-fossil carbon in the OC and/or EC components are also presented where these were measured.…”

Section: Compound-specific 14 C Determinationsmentioning

confidence: 99%

The application of carbon-14 analyses to the source apportionment of atmospheric carbonaceous particulate matter: a review

Heal

2013

Anal Bioanal Chem

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Organic carbon (OC) and elemental carbon (EC) together constitute a substantial proportion of airborne particulate matter (PM). Insight into the sources of this major contributor to PM is important for policies to mitigate the impact of PM on human health and climate change. In recent years measurement of the abundance of the radioisotope of carbon ((14)C) in samples of PM by accelerator mass spectrometry has been used to help quantify the relative contributions from sources of fossil carbon and contemporary carbon. This review provides an introduction to the different sources of carbon within PM and the role of (14)C measurements, a description of the preparation of PM samples and of the instrumentation used to quantify (14)C, and a summary of the results and source apportionment methods reported in published studies since 2004. All studies report a sizable fraction of the carbonaceous PM as of non-fossil origin. Even for PM collected in urban locations, the proportions of non-fossil carbon generally exceed 30%; typically the proportion in urban background locations is around 40-60% depending on the local influence of biomass burning. Where values have been measured directly, proportions of non-fossil carbon in EC are lower than in OC, reflecting the greater contribution of fossil-fuel combustion to EC and the generally small sources of contemporary EC. Detailed source apportionment studies point to important contributions from biogenic-derived secondary OC, consistent with other evidence of a ubiquitous presence of heavily oxidized background secondary OC. The review concludes with some comments on current issues and future prospects, including progress towards compound-class and individual-compound-specific (14)C analyses.

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“…The fine particles discussed here can travel deep into the human respiratory system and, for the smallest particles, potentially enter the bloodstream, thus exposing people to both particles and the particle-bound compounds (Geiser et al, 2005). To solve these problems, the first thing we should clarify is the releasing source of size-specific PAHs as well as their transport characteristics in the human respiratory system (Chen and Liao, 2006;Sheesley et al, 2009). …”

Section: Introductionmentioning

confidence: 99%

Size distributions of polycyclic aromatic hydrocarbons in urban atmosphere: sorption mechanism and source contributions to respiratory deposition

et al. 2016

Atmos. Chem. Phys.

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Abstract. In order to better understand the particle size distribution of polycyclic aromatic hydrocarbons (PAHs) and their source contribution to human respiratory system, sizeresolved PAHs have been studied in ambient aerosols at a megacity Shanghai site during a 1-year period (2012)(2013). The results showed the PAHs had a bimodal distribution with one mode peak in the fine-particle size range (0.4-2.1 µm) and another mode peak in the coarse-particle size range (3.3-9.0 µm). Along with the increase in ring number of PAHs, the intensity of the fine-mode peak increased, while the coarsemode peak decreased. Plotting of log(PAH / PM) against log(D p ) showed that all slope values were above −1, suggesting that multiple mechanisms (adsorption and absorption) controlled the particle size distribution of PAHs. The total deposition flux of PAHs in the respiratory tract was calculated as being 8.8 ± 2.0 ng h −1 . The highest lifetime cancer risk (LCR) was estimated at 1.5 × 10 −6 , which exceeded the unit risk of 10 −6 . The LCR values presented here were mainly influenced by accumulation mode PAHs which came from biomass burning (24 %), coal combustion (25 %), and vehicular emission (27 %). The present study provides us with a mechanistic understanding of the particle size distribution of PAHs and their transport in the human respiratory system, which can help develop better source control strategies.

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Source apportionment of elevated wintertime PAHs by compound-specific radiocarbon analysis

Cited by 46 publications

References 51 publications

The sequestration sink of soot black carbon in the Northern European Shelf sediments

The sequestration sink of soot black carbon in the Northern European Shelf sediments

The application of carbon-14 analyses to the source apportionment of atmospheric carbonaceous particulate matter: a review

Size distributions of polycyclic aromatic hydrocarbons in urban atmosphere: sorption mechanism and source contributions to respiratory deposition

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