Određivanje porekla PM2,5 frakcije aerosola u graničnoj zoni urbanog područja Beograda primenom komplementarnih statističkih metoda
Determining the origin of pm2.5 aerosol fraction in a belgrade urban boundary area using complemental statistical methods
Докторанд
Todorović, MarijaМентор
Ignjatović, LjubišaЧланови комисије
Vukelić, NikolaRadenković, Mirjana
Метаподаци
Приказ свих података о дисертацијиСажетак
U ovom radu analizirani su elementni i jonski sastav PM2,5 frakcije aerosola uzorkovanih
tokom perioda Maj 2014 – Maj 2015. godine na rubu urbane teritorije Beograda. Masene
koncentracije 19 elemenata (Al, Si, P, S, Cl, K, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn,
Br, As, Sr, Ba, Pb) u sastavu PM2,5 izmerene su PIXE (Particle Induced X-ray Emission)
metodom, dok su koncentracije tri najzastupljenija jona (NH4+, NO3-, SO42-) određene
metodom jonske hromatografije. Primenom receptorskog modela PMF (Positive Matrix
Factorisation) modela, na osnovu hemijskog sastava PM2,5, određene su dominantne grupe
izvora zagađenja i njihovi doprinosi. Obrasci atmosferske cirkulacije – lokalne i regionalne –
i njihov uticaj na doprinose identifikovanih izvora, kao i na masene koncentracije gasova
prekursora neorganskih jona (NO2 i SO2), ispitani su kombinacijom niza receptorskih modela.
Rezultati su pokazali da, iako postoji trend opadanja posmatrano u periodu od sedam godina,
masene koncentracije komp...onenata antropogenog porekla u sastavu PM2,5, poput S, K i Pb,
i dalje su relativno visoke, naročito tokom grejne sezone. Osim Ca i Ti, masene koncentracije
svih elemenata bile su pod manjim ili većim uticajem antropogenih aktivnosti, koji je takođe
izraženiji tokom grejne sezone. Neutralizacioni odnos sugerisao je kiselost PM2,5 na
posmatranoj teritoriji, dok je nazastupljeniji jon bio SO42-.
Identifikovano je pet dominantnih grupa izvora PM2,5: sagorevanje biomase, saobraćaj,
sekundarni sulfati, lokalno sagorevanje fosilnih goriva sa nitratima i resuspenzija prašine.
Najveće relativne doprinose pokazali su sagorevanje fosilnih goriva sa nitratima i sekundarni
sulfati, dok je doprinos emisija iz sagorevanja biomase bio znatno niži. Analize uticaja
lokalnih i dugometnih obrazaca atmosferske cirkulacije na doprinose izvora sugerisale su
dominantno lokalno poreklo sagorevanja biomase i fosilnih goriva, formacije nitrata i
saobraćaja. Pokazano je takođe da su sekundarni sulfati i resuspenzija prašine (zemljišne
prašine ili peska) pod značajnim uticajem regionalinih i prekograničnih emisija. Interesantno
je da su karakteristični meteorološki uslovi tokom merne kampanje – izuzetno visoka
precipitacija i posledične poplave – naglasili značajnost uticaja emisija (SO2) iz regionalnih
termoelektrana i termoelektrana na Balkanu na kvalitet vazduha u Beogradu. Pored uticaja
resuspenzije poljoprivrednog zemljišta, predviđanja NOAA HYSPLIT modela ukazala su na
doprinose peska transportovanog iz Saharske pustinje kao i iz oblasti istočno od Kaspijskog
mora. Procena zdravstvenih uticaja PM2,5 sugerisala je da su najštetniji uticaji emisija iz
lokanih procesa sagorevanja i sekundarnih sulfata, mada su detaljnija ispitivanja neophodna
kako na epidemiološkoj tako i na toksikološkoj bazi.
The subject of this dissertation is the analysis of the elemental and ionic composition of the
PM2.5 aerosol fraction sampled in May 2014 - May 2015 on the outskirts of the Belgrade
urban area. Mass concentrations of 19 elements (Al, Si, P, S, Cl, K, Ca, Sc, Ti, V, Cr, Mn,
Fe, Co, Ni, Cu, Zn, Br, As, Sr, Ba, Pb), components of PM2.5, were measured by the PIXE
method (Particle Induced X-ray analysis), while concentrations of the three major ions
(NH4+, NO3-, SO42-) were determined by ion chromatography. Based on the chemical
composition of PM2.5, the dominant groups of pollution sources and their contributions were
determined using the PMF (Positive Matrix Factorization) receptor model. Atmospheric
circulation patterns, local and regional, and their influence on the contributions of identified
sources and mass concentrations of PM2,5 gaseous precursors (NO2 and SO2) were examined
with a combination of several receptor models.
The results showed that although there is a declining trend i...n the concentrations of
anthropogenic components in PM2.5 (observed over a period of seven years), mass
concentrations of some of them, such as S, K and Pb, are still relatively high, especially
during the heating season. Apart from Ca and Ti, the concentrations of all elements were
influenced by anthropogenic activities, which were more pronounced during the heating
season. The neutralization coefficient suggested that PM2.5 within the examined territory
was mainly acidic, while the most abundant ion was SO42-.
Five dominant groups of PM2.5 sources have been identified: biomass burning, traffic,
secondary sulfates, local combustion of fossil fuels mixed with nitrates, and dust
resuspension. Combustion of fossil fuels with nitrates and secondary sulfates showed the
largest relative contributions, while the contribution of emissions from biomass burning was
lower. Analyses of the influence of local and long-term patterns of atmospheric circulation
on the contribution of these sources suggested the dominant local origin of biomass burning
and fossil fuel combustion, nitrate formation processes, and traffic. It has also been shown
that secondary sulfates and dust resuspension were significantly affected by regional and
transboundary emissions. Specific meteorological conditions that marked the measurement
campaign (extremely high precipitation and consequential floods) emphasized the impact of
SO2 - emitted from thermal power plants in Serbia and the Balkan region - on Belgrade air
quality. Predictions from NOAA HYSPLIT model indicated the contribution of sand
transported from the Saharan and Turkmenistan deserts in addition to the likely impact of
resuspension of regional agricultural soil. Analysis of relations between the health impacts
of PM2.5 on the population of Belgrade and the identified sources’ contributions suggested
that the most harm was caused by emissions from local combustion processes and secondary
sulfates. More detailed studies on this subject are necessary using both an epidemiologicaland toxicological approach.
Факултет:
Универзитет у Београду, Факултет за физичку хемијуДатум одбране:
29-12-2020Пројекти:
- Истраживање климатских промена и њиховог утицаја на животну средину - праћење утицаја, адаптација и ублажавање (RS-MESTD-Integrated and Interdisciplinary Research (IIR or III)-43007)