Abstract
We applied stable carbon isotope ratio (^(13)C/^(12)C) and radiocarbon (^(14)C) analysis for the quantification of three main aerosol sources (coal, biomass and liquid fossil fuel derived aerosol emissions). Submicron aerosol samples (PM1) were collected from 27^(th) October, 2014 to 19^(th) January, 2015 at a suburban site of Vilnius city (Lithuania). To determine fossil and non-fossil contributions to submicron carbonaceous aerosol particles, ^(14)C measurements of total carbon (TC) were performed using single stage accelerator mass spectrometer (SSAMS, NEC, USA). The concentrations of TC and δ^(13)C in PM_1 fraction were measured using elemental analyzer interfaced to isotope ratio mass spectrometer (EA-IRMS). The TC concentration during measurement period ranged from 1.3 to 9.6 μg m^(-3). The variation of TC concentrations can be explained by the influence of long-range transport and dispersion properties of the boundary layer (mixed layer depth). We found that biomass-derived aerosol sources are prevailing in Vilnius during wintertime and ranged from 57% to 84% of total carbonaceous aerosol fraction. Applying isotope mass balance calculations the traffic emissions were estimated to be 15 ± 7% and coal combustion made up 14 ± 9% in PM_1. To provide better information about the pollution sources, the carbon isotope analysis along air mass transport pattern was performed. Our results demonstrated that the high contribution to PM_1 from coal burning (up to 40%) was observed for air masses transported from highly industrialized Western Europe regions. Combination of stable carbon isotope ratio with the radiocarbon data allow to distinguish coal from liquid fossil fuel in the aerosol particle emissions.
Highlights
Fine aerosol particles have a significant effect on the climate change, direct and indirect radiative forcing, visibility and human health (Watson, 2002; Forster et al, 2007; Mauderly and Chow, 2008)
Our results demonstrated that the high contribution to PM1 from coal burning was observed for air masses transported from highly industrialized Western Europe regions
Sector 4 represents eastern air masses coming from Belarus, northern Ukraine and Russia. 2–4 sectors were classified as “polluted” sectors characterized by various types of carbonaceous pollution sources such as petrol and diesel emissions, oil USA-SSAMS, fraction of modern carbon (fM) 0.74 ± 0.01 0.79 ± 0.01 0.87 ± 0.01 0.76 ± 0.01
Summary
Fine aerosol particles (particles having the aerodynamic diameter < 1 μm, PM1) have a significant effect on the climate change, direct and indirect radiative forcing, visibility and human health (Watson, 2002; Forster et al, 2007; Mauderly and Chow, 2008). Distinguishing fossil fuel and biomass burning sources is necessary to develop abatement strategies for more efficient control of carbonaceous aerosol particle pollution. Different aerosol sources have a specific stable carbon isotopic composition (13C/12C). Recent studies demonstrated significant difference in δ13C values between coal (δ13C(coal) = –24.5‰) and liquid fossil fuel (δ13C(liquid fossil fuel) = –28‰) (Górka et al, 2009; Garbaras et al, 2015;) This isotope ratios differences can be used for identification of specific aerosol particle sources. Ceburnis et al (2011) used a dual isotope (14C and 13C) method for quantifying biogenic marine and terrestrial organic aerosol sources. Our main objective was to distinguish coal, biomass and liquid fossil fuel-derived PM1 aerosol particles in the Vilnius city applying the stable carbon isotope ratio and radiocarbon analysis
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