Source apportionment of carbonaceous aerosols in diverse atmospheric environments of China by dual-carbon isotope method

2021 ◽  
pp. 150654
Author(s):  
Mengren Li ◽  
Min Hu ◽  
Jennifer Walker ◽  
Pan Gao ◽  
Xin Fang ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Carbon Isotope ◽  
Carbonaceous Aerosols ◽  
Isotope Method

scholarly journals Six-year source apportionment of submicron organic aerosols from near-continuous measurements at SIRTA (Paris area, France)

2019 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Ambient Air ◽  
Carbonaceous Aerosols ◽  
Time Resolved ◽  
Pronounced Increase ◽  
Paris Area ◽  
Multi Wavelength ◽  
High Concentrations

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly-time resolved year-round characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of Aerosol Chemical Speciation Monitor (ACSM) and multi-wavelength aethalometer from November 2011 to March 2018 at a background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase of LO-OOA concentrations and contributions (50–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely high concentrations and OA contributions (32–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter, and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about 200 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil fuel and biomass burning black carbon components), and no trend for LO-OOA over the 6+-year investigated period.

scholarly journals Six-year source apportionment of submicron organic aerosols from near-continuous highly time-resolved measurements at SIRTA (Paris area, France)

2019 ◽  
Vol 19 (23) ◽  
pp. 14755-14776 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Ambient Air ◽  
Carbonaceous Aerosols ◽  
Time Resolved ◽  
Pronounced Increase ◽  
Paris Area ◽  
Range Transport ◽  
High Concentrations

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly time-resolved long-term characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of an aerosol chemical speciation monitor (ACSM) and a multiwavelength Aethalometer from November 2011 to March 2018 at a peri-urban background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18 %–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase in LO-OOA concentrations and contributions (50 %–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely, high concentrations and OA contributions (32 %–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about −175 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil-fuel and biomass-burning black carbon components) and no statistically significant trend for LO-OOA over the 6-year investigated period.

scholarly journals Year-round radiocarbon-based source apportionment of carbonaceous aerosols at two background sites in South Asia

2012 ◽  
Vol 117 (D10) ◽  
pp. n/a-n/a ◽  
Author(s):  
Rebecca J. Sheesley ◽  
Elena Kirillova ◽  
August Andersson ◽  
Martin Kruså ◽  
P. S. Praveen ◽  
...  
Keyword(s):  
South Asia ◽  
Source Apportionment ◽  
Carbonaceous Aerosols

Dual carbon isotope characterization of total organic carbon in wintertime carbonaceous aerosols from northern India

2016 ◽  
Vol 121 (9) ◽  
pp. 4797-4809 ◽  
Author(s):  
Srinivas Bikkina ◽  
August Andersson ◽  
M. M. Sarin ◽  
R. J. Sheesley ◽  
E. Kirillova ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Total Organic Carbon ◽  
Carbon Isotope ◽  
Carbonaceous Aerosols ◽  
Northern India

scholarly journals Accuracy and precision of <sup>14</sup>C-based source apportionment of organic and elemental carbon in aerosols using the Swiss_4S protocol

2015 ◽  
Vol 8 (4) ◽  
pp. 3933-3965 ◽  
Author(s):  
G. O. Mouteva ◽  
S. M. Fahrni ◽  
G. M. Santos ◽  
J. T. Randerson ◽  
Y. L. Zhang ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Elemental Carbon ◽  
Small Sample ◽  
Mitigation Strategies ◽  
Pure Oxygen ◽  
Carbonaceous Aerosols ◽  
Carbon Fraction ◽  
Fossil Carbon ◽  
Vacuum Line ◽  
Set Up

Abstract. Aerosol source apportionment remains a critical challenge for understanding the transport and aging of aerosols, as well as for developing successful air pollution mitigation strategies. The contributions of fossil and non-fossil sources to organic carbon (OC) and elemental carbon (EC) in carbonaceous aerosols can be quantified by measuring the radiocarbon (14C) content of each carbon fraction. However, the use of 14C in studying OC and EC has been limited by technical challenges related to the physical separation of the two fractions and small sample sizes. There is no common procedure for OC/EC 14C analysis, and uncertainty studies have largely focused on the precision of yields. Here, we quantified the uncertainty in 14C measurement of aerosols associated with the isolation and analysis of each carbon fraction with the Swiss_4S thermal-optical analysis (TOA) protocol. We used an OC/EC analyzer (Sunset Laboratory Inc., OR, USA) coupled to vacuum line to separate the two components. Each fraction was thermally desorbed and converted to carbon dioxide (CO2) in pure oxygen (O2). On average 91% of the evolving CO2 was then cryogenically trapped on the vacuum line, reduced to filamentous graphite, and measured for its 14C content via accelerator mass spectrometry (AMS). To test the accuracy of our set-up, we quantified the total amount of extraneous carbon introduced during the TOA sample processing and graphitization as the sum of modern and fossil (14C-depleted) carbon introduced during the analysis of fossil reference materials (adipic acid for OC and coal for EC) and contemporary standards (oxalic acid for OC and rice char for EC) as a function of sample size. We further tested our methodology by analyzing five ambient airborne particulate matter (PM2.5) samples with a range of OC and EC concentrations and 14C contents in an interlaboratory comparison. The total modern and fossil carbon blanks of our set-up were 0.8 ± 0.4 and 0.67 ± 0.34 μg C, respectively, based on multiple measurements of ultra-small samples. The Swiss_4S protocol and the cryo-trapping contributed 0.37 ± 0.18 μg of modern carbon and 0.13 ± 0.07 μg of fossil carbon to the estimated blanks, with consistent estimates obtained for the two laboratories. There was no difference in the background correction between the OC and EC fractions. Our set-up allowed us to efficiently isolate and trap each carbon fraction with the Swiss_4S protocol and to perform 14C analysis of ultra-small OC and EC samples with high accuracy and low 14C blanks.

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