Title Study of aerosol particle origin and dispersion by isotope ratio mass spectrometry /
Translation of Title Atmosferos aerozolio dalelių kilmės ir sklaidos tyrimas stabilių izotopų masių spektrometrijos metodu.
Authors Garbaras, Andrius
Full Text Download
Pages 33
Keywords [eng] aerosol particle ; transport ; d13C
Abstract [eng] The development of industry, transport, agriculture and power engineering inevitably create problems related to the impact of generated waste on the environment as well as other undesirable processes. The atmosphere is the main component of the Earth’s climate system because changes occurring due to the human economic activity result in serious environmental impacts in all components of the ecosystem as well as the Earth’s climate self-regulation system is disturbed. The objective of this work was to investigate the origin, sources and formation of organic compounds and black carbon in atmospheric aerosol particles and to develop new research methods. To attain this objective the following tasks have been formulated: Development of the identification method for the aerosol origin and source by investigating the carbon isotope mass ratios, illustration of possibilities of the carbon isotope ratio method by identifying the aerosol particle origin during the air mass long-range transport at the Preila Environmental pollution research station, investigation of variation of the black carbon amount in aerosol particles in the diesel engine exhaust depending on the engine working parameters and fuel composition, investigation of the carbon isotope ratio variation in natural aerosol depending on the aerosol particle size distribution, determination of the partial contribution of natural and anthropogenic particles in aerosol by investigation of stable carbon and radiocarbon isotope ratio changes during continental and marine air mass transport. In conclusions it is shown that: The carbon isotope ratio in anthropogenic origin aerosol particles corresponds to the isotope ratio of burnt fuel (biomass and fossil fuel), and this parameter is suitable for identification of the aerosol particle source. In the aerosol particles from the environment in the size range up to 1 μm, vegetative organic carbon is prevailing. The largest organic and elemental carbon ratio value (OA/EA=13.1) was observed in the accumulation mode, in the particle size interval from 0.18 µm to 0.32 µm. Such value is typical of background localities. δ13C values of elemental carbon in the accumulation mode varied from -22,9 ‰ to -26,3 ‰, while organic carbon δ13C values were about -28 ‰. From the carbon isotope ratio values it has been determined that the elemental carbon precursors in aerosol particles were from burning products, while the source of organic carbon was volatile organic compounds from vegetation; in the aerosol particles larger than 1μm the carbonate component is observed. In the range of all sizes the carbon isotope ratio of vegetative organic origin component does not change. By combining aerosol mass and isotope ratio mass spectrometry methods it has been determined that in aerosol particles of the accumulation mode (in the size interval from 0.056 to 1 μm) from 80 % to 90 % of carbon is of organic (vegetative) origin; the measured δ13C values in diesel fuel and diesel fuel with 10 % and 40 % of ethanol varied from -29 ‰ to -30,7 ‰. It has been determined that the isotope fractionation between fuel and aerosol particles was 1.3 ‰ and did not depend on the engine load and revolutions per minute, when diesel fuel with 40 % of ethanol was used. Such fractionation factor between this type of fuel and aerosol particles indicates that ethanol did not participate in the aerosol particle formation; the method of identifying the aerosol particles from marine, biomass and continental fossil fuel burning products has been developed and experimentally realized. It has been shown that in clean air over the North Eastern Atlantic Ocean the marine biogenic submicron carbonaceous particle source dominates (80 %). In continental air masses on average there are 30 % of marine aerosol particles, 40 % from fossil fuel and 30 % from biomass burning aerosol particles.
Type Summaries of doctoral thesis
Language English
Publication date 2011