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One-Year-Long Continuous and Synchronous Data Set of Fossil Carbon in Atmospheric PM2.5 and Carbon Dioxide in Debrecen, Hungary

Published online by Cambridge University Press:  23 February 2016

István Major ,
Enikő Furu ,
László Haszpra ,
Zsófia Kertész  and
Mihály Molnár
István Major*
Affiliation:
Hertelendi Laboratory of Environmental Studies, MTA ATOMKI, Bem tér 18/c, H-4026 Debrecen, Hungary
Enikő Furu
Affiliation:
Laboratory of Ion Beam Applications, MTA ATOMKI, Debrecen, Hungary
László Haszpra
Affiliation:
Hungarian Meteorological Service, Budapest, Hungary MTA Research Centre for Astronomy and Earth Sciences, Sopron, Hungary
Mihály Molnár
Affiliation:
Hertelendi Laboratory of Environmental Studies, MTA ATOMKI, Bem tér 18/c, H-4026 Debrecen, Hungary
*
2. Corresponding author. Email: [email protected].
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Abstract

Radiocarbon investigation of atmospheric PM2.5 aerosol synchronized with 14CO2 observations began in Debrecen in the winter of 2010. The aim of the study was to determine the contemporary and fossil carbon fractions in the aerosol and to set them against the fossil CO2 excess data referring to the same period. The mass of the collected PM2.5 mode on prebaked quartz filters was determined gravimetrically, while its total carbon mass was calculated from the pressure of CO2 gas produced after the combustion of the filters. As a result of the applied sampling and preparation method, the stable, nonvolatile carbon forms were principally studied. 14C measurements of the tiny aerosol bulk samples were performed using the EnvironMICADAS accelerator mass spectrometer at ATOMKI. The sample preparation method was tested using several blanks, standards, and real samples. Test results showed good reproducibility for the applied aerosol sample preparation and accelerator mass spectrometry (AMS) 14C analyses. Atmospheric fossil CO2 excess data were calculated according Levin et al. (2003), using the 14C results of collected CO2 samples measured by the gas proportional counting system at ATOMKI. Mass concentration of PM10 involving the PM2.5 mode in the city air exceeded the daily average of 50 μg/m3 (24-hr limit value in the EU) several times in 2011, mainly during the winter. The results showed that recently derived carbon most likely from domestic wood burning was causing the elevated carbon mass concentration of PM2.5 in Debrecen at the time. In the course of the 1-yr-long continuous and systematic comparison of fossil carbon mass concentration of PM2.5 mode and mole fraction of fossil excess of atmospheric CO2, similar and synchronous trends were observed during the studied period in Debrecen.

Type
Articles
Information
Radiocarbon , Volume 57 , Issue 5 , 2015 , pp. 991 - 1002
Copyright
Copyright © 2015 The Arizona Board of Regents on behalf of the University of Arizona 

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References

AQEG (Air Quality Expert Group). 2005. Particulate matter in the United Kingdom. Second report of the AQEG, UK Department for Environment, Food and Rural Affairs. PB10580, London.Google Scholar
Bench, G, Fallon, S, Schichtel, B, Malm, W, McDade, C. 2007. Relative contributions of fossil and contemporary carbon sources to PM2.5 aerosols at nine Interagency Monitoring for Protection of Visual Environments (IMPROVE) network sites. Journal of Geophysical Research 112:D10205.Google Scholar
Borbély-Kiss, I, Kertész, Zs, Koltay, E, Szabó, Gy, Tar, K. 1999. Composition of urban and rural aerosol samples collected in the Great Hungarian Plain. Nuclear Instruments and Methods in Physics Research B 150(1–4):339–44.CrossRefGoogle Scholar
Burr, GS, Jull, AJT. 2009. Accelerator mass spectrometry for radiocarbon research. In: Gross, ML, Caprioli, R, editors. Encyclopedia of Mass Spectrometry. Volume 5. Amsterdam: Elsevier. p 656–69.Google Scholar
Cachier, H. 1998. Carbonaceous combustion aerosols. In: Harrison, RM, van Grieken, R, editors. Atmospheric Particles. IUPAC series on analytical and physical chemistry of environmental systems, Volume 5. Chichester: John Wiley & Sons. p 295–348.Google Scholar
Chow, JC, Watson, JG. 2002. PM2.5 carbonate concentrations at regionally representative Interagency Monitoring of Protected Visual Environment sites. Journal of Geophysical Research 107:8344.Google Scholar
Chow, JC, Watson, JG, Chen, LWA, Arnott, WP, Moosmuller, H. 2004. Equivalence of elemental carbon by thermal/optical reflectance and transmittance with different temperature protocols. Environmental Science & Technology 38(16):4414–22.CrossRefGoogle ScholarPubMed
Clayton, GD, Arnold, JR, Patty, FA. 1955. Determination of sources of particulate atmospheric carbon. Science 122(3173):751–3.Google Scholar
Csongor, É, Hertelendi, E. 1986. Low-level counting facility for 14C dating. Nuclear Instruments and Methods in Physics Research B 17(5–6):493–5.CrossRefGoogle Scholar
Csongor, É, Szabó, I, Hertelendi, E. 1982. Preparation of counting gas of proportional counters for radiocarbon dating. Radiochemical and Radioanalytical Letters 55(5–6):303–7.Google Scholar
Currie, LA. 2000. Evolution and multidisciplinary frontiers of 14C aerosol science. Radiocarbon 42(1):115–26.CrossRefGoogle Scholar
Currie, LA, Stafford, TW, Sheffield, AE, Klouda, GA, Wise, SA, Fletcher, RA, Donahue, DJ, Jull, AJT, Linick, TW. 1989. Microchemical and molecular dating. Radiocarbon 31(3):448–63.Google Scholar
Endo, M, Yamamoto, N, Yoshinaga, J, Yanagisawa, Y, Endo, O, Goto, S, Yoneda, M, Shibata, Y, Morita, M. 2004. 14C measurement for size fractionated airborne particulate matters. Atmospheric Environment 38(36):6263–7.Google Scholar
Environmental Program of Debrecen. 2009–2014. Plánum 97 Kft. 2009. Debrecen. In Hungarian.Google Scholar
Heal, MR, Naysmith, P, Cook, GT, Xu, S, Duran, TR, Harrison, RM. 2011. Application of 14C analyses to source apportionment of carbonaceous PM2.5 in the UK. Atmospheric Environment 45(36):2341–8.CrossRefGoogle Scholar
Heintzenberg, J. 1989. Fine particles in the global troposphere: a review. Tellus B 41:149–60.CrossRefGoogle Scholar
Hertelendi, E. 1990. Developments of methods and equipment for isotope analytical purposes and their applications [CSc thesis]. Hungarian Academy of Sciences. In Hungarian.Google Scholar
Huang, J, Kang, S, Shen, C, Cong, Z, Liu, K, Wang, W, Liu, L. 2010. Seasonal variations and sources of ambient fossil and biogenic-derived carbonaceous aerosols based on 14C measurements in Lhasa, Tibet. Atmospheric Research 96(4):553–9.Google Scholar
Krivácsy, Z, Sávári, Z, Temesi, D, Baltensperger, U, Nyeki, S, Weingartner, E, Kleefeld, S, Jennings, SG. 2001. Role of organic and black carbon in the chemical composition of atmospheric aerosol at European background sites. Atmospheric Environment 35(36):6231–44.CrossRefGoogle Scholar
Künzli, N, Kaiser, R, Medina, S, Studnicka, M, Chanel, O, Filliger, P, Herry, M, Horak, F Jr, Puybonnieux-Texier, V, Quénel, P, Schneider, J, Seethaler, R, Vergnaud, JC, Sommer, H. 2000. Public-health impact of outdoor and traffic-related air pollution: a European assessment. The Lancet 356(9232):795–801.Google Scholar
Larssen, S, Sluyter, R, Helmis, C. 1999. Criteria for EUROAIRNET, the EEA air quality monitoring and information network. Technical Report NO12.Google Scholar
Levin, I, Kromer, B, Schmidt, M, Sartorius, H. 2003. A novel approach for independent budgeting of fossil fuel CO2 over Europe by 14CO2 observations. Geophysical Research Letters 30(23):2194.Google Scholar
Molnár, A, Mészáros, E, Hansson, HC, Karlsson, H, Gelencsér, A, Kiss, Gy, Kriváncsy, Z. 1999. The importance of organic and elemental carbon in the fine atmospheric aerosol particles. Atmospheric Environment 33:2745–50.CrossRefGoogle Scholar
Molnár, M, Bujtás, T, Svingor, É, Futó, I, Svetlik, I. 2007. Monitoring of atmospheric excess 14C around Paks Nuclear Power Plant, Hungary. Radiocarbon 49(2):1031–43.CrossRefGoogle Scholar
Molnár, M, Haszpra, L, Svingor, É, Major, I, Svetlik, I. 2010a. Atmospheric fossil fuel CO2 measurement using a field unit in a central European city during the winter of 2008/09. Radiocarbon 52(2):835–45.CrossRefGoogle Scholar
Molnár, M, Major, I, Haszpra, L, Svetlik, I, Svingor, É, Veres, M. 2010b. Fossil fuel CO2 estimation by atmospheric 14C measurement and CO2 mixing ratios in the city of Debrecen, Hungary. Journal of Radioanalytical and Nuclear Chemistry 286(2):471–6.Google Scholar
Molnár, M, Janovics, R, Major, I, Orsovszki, J, Gönczi, R, Veres, M, Leonard, AG, Castle, SM, Lange, TE, Wacker, L, Hajdas, I, Jull, AJT. 2013a. Status report of the new AMS 14C sample preparation lab of the Hertelendi Laboratory of the Environmental Studies (Debrecen, Hungary). Radiocarbon 55(2–3):665–76.Google Scholar
Molnár, M, Rinyu, L, Veres, M, Seiler, M, Wacker, L, Synal, HA. 2013b. EnvironMICADAS: a mini 14C AMS with enhanced gas ion source interface in the Hertelendi Laboratory of Environmental Studies (HEKAL), Hungary. Radiocarbon 55(2–3):338–44.Google Scholar
Novakov, T, Hegg, DA, Hobbs, PV. 1997. Airborne measurements of carbonaceous aerosols on the East Coast of the United States. Journal of Geophysical Research Atmospheres 102(D25):30,023–30.Google Scholar
Pedersen, M, Giorgis-Allemand, L, Bernard, C, Aguilera, I, Andersen, AMN, Ballester, F, Beelen, RMJ, Chatzi, L, Cirach, M, Danileviciute, A, Dedele, A, van Eijsden, M, Estarlich, M, Fernández-Somoano, A, Fernández, MF, Forastiere, F, Gehring, U, Grazuleviciene, R, Gruzieva, O, Heude, B, Hoek, G. 2013. Ambient air pollution and low birth weight: a European cohort study (ESCAPE). The Lancet Respiratory Medicine 1(9):695–704.CrossRefGoogle ScholarPubMed
Pöschl, U. 2005. Atmospheric aerosols: composition, transformation, climate and health effects. Angewandte Chemie 44:7520–40.Google ScholarPubMed
Putaud, JP, Van Dingenen, R, Alastuey, A, Bauer, H, Birmili Cyrys, J, Flentje, H, Fuzzi, S, Gehrig, R, Hansson, HC, Harrison, RM, Herrmann, H, Hitzenberger, R, Hüglin, C, Jones, AM, Kasper-Giebl, A, Kiss, G, Kousa, A, Kuhlbusch, TAJ, Löschau, G, Maenhaut, W, Molnar, A, Moreno, T, Pekkanen, J, Perrino, C, Pitz, M, Puxbaum, H, Querol, X, Rodriguez, S, Salma, I, Schwarz, J, Smolik, J, Schneider, J, Spindler, G, ten Brink, H, Tursic, J, Viana, M, Wiedensohler, A, Raes, F. 2010. A European aerosol phenomenology – 3: Physical and chemical characteristics of particulate matter from 60 rural, urban, and kerbside sites across Europe. Atmospheric Environment 44(10):1308–20.Google Scholar
Ramanathan, V, Ramana, MV, Roberts, G, Kim, D, Corrigan, C, Chung, C, Winker, D. 2007. Warming trends in Asia amplified by brown cloud solar absorption. Nature 448(7153):575–8.Google Scholar
Rinyu, L, Molnár, M, Major, I, Nagy, T, Veres, M, Kimák, Á, Wacker, L, Synal, H-A. 2013. Optimization of sealed tube graphitization method for environmental 14C studies using MICADAS. Nuclear Instruments and Methods in Physics Research B 294(1):270–5.CrossRefGoogle Scholar
Rogge, WF, Hildemann, LM, Mazurek, MA, Cass, GR, Simoneit, BRT. 1993. Sources of fine organic aerosol. 4. Particulate abrasion products from leaf surfaces of urban plants. Environmental Science and Technology 27(4):2700–11.Google Scholar
Saxena, P, Hildemann, LM, McMurry, PH, Seinfeld, JH. 1995. Organics alter hygroscopic behavior of atmospheric particles. Journal of Geophysical Research 100(D9):18,755–70.Google Scholar
Stuiver, M, Polach, H. 1977. Discussion: reporting of 14C data. Radiocarbon 19(3):355–63.CrossRefGoogle Scholar
Szidat, S, Jenk, TM, Gaggeler, HW, Synal, H-A, Fisseha, R, Baltensperger, U, Kalberer, M, Samburova, V, Reimann, S, Kasper-Giebl, A, Hajdas, I. 2004. Radiocarbon (14C)-deduced biogenic and anthropogenic contributions to organic carbon (OC) of urban aerosols from Zurich, Switzerland. Atmospheric Environment 38(24):4035–44.Google Scholar
Szidat, S, Jenk, TM, Synal, H-A, Kalberer, M, Wacker, L, Hajdas, I, Kasper-Giebl, A, Baltensperger, U. 2006. Contributions of fossil fuel, biomass-burning, and biogenic emissions to carbonaceous aerosols in Zurich as traced by 14C. Journal of Geophysical Research 111:D07206.CrossRefGoogle Scholar
Szidat, S, Ruff, M, Perron, N, Wacker, L, Synal, HA, Hallquist, M, Shannigrahi, AS, Yttri, KE, Dye, C, Simpson, D. 2009. Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Goteborg, Sweden. Atmospheric Chemistry and Physics 9:1521–35.Google Scholar
Tanner, RL, Parkhurst, WJ, Valente, ML, Phillips, WD. 2004. Regional composition of PM2.5 aerosols measured at urban, rural and “background” sites in the Tennessee valley. Atmospheric Environment 38(20):3143–53.Google Scholar
Turpin, BJ, Saxena, P, Andrews, E. 2000. Measuring and simulating particulate organics in the atmosphere: problems and prospects. Atmospheric Environment 34(18):2983–3013.Google Scholar
Uchrin, G, Hertelendi, E. 1992. Development of a reliable differential Carbon-14 sampler for environmental air and NPP stack monitoring. Final Report of the OMFB contract No. 001.Google Scholar
Wacker, L, Christl, M, Synal, H-A. 2010. Bats: a new tool for AMS data reduction. Nuclear Instruments and Methods in Physics Research B 268(7–8):976–9.Google Scholar