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Source Apportionment of Aerosols by 14C Measurements in Different Carbonaceous Particle Fractions

Published online by Cambridge University Press:  18 July 2016

S Szidat ,
T M Jenk ,
H W Gäggeler ,
H-A Synal ,
R Fisseha ,
U Baltensperger ,
M Kalberer ,
V Samburova ,
L Wacker  and
M Saurer
...Show all authors
S Szidat
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, CH-3012 Bern, Switzerland.
T M Jenk
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, CH-3012 Bern, Switzerland. Paul Scherrer Institut (PSI), CH-5232 Villigen, Switzerland.
H W Gäggeler*
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, CH-3012 Bern, Switzerland. Paul Scherrer Institut (PSI), CH-5232 Villigen, Switzerland.
H-A Synal
Affiliation:
Paul Scherrer Institut (PSI), c/o Institute for Particle Physics, ETH Hönggerberg, CH-8093 Zürich, Switzerland.
R Fisseha
Affiliation:
Paul Scherrer Institut (PSI), CH-5232 Villigen, Switzerland.
U Baltensperger
Affiliation:
Paul Scherrer Institut (PSI), CH-5232 Villigen, Switzerland.
M Kalberer
Affiliation:
Laboratory of Organic Chemistry, ETH Hönggerberg, CH-8093 Zürich, Switzerland.
V Samburova
Affiliation:
Laboratory of Organic Chemistry, ETH Hönggerberg, CH-8093 Zürich, Switzerland.
L Wacker
Affiliation:
Institute for Particle Physics, ETH Hönggerberg, CH-8093 Zürich, Switzerland.
M Saurer
Affiliation:
Paul Scherrer Institut (PSI), CH-5232 Villigen, Switzerland.
M Schwikowski
Affiliation:
Paul Scherrer Institut (PSI), CH-5232 Villigen, Switzerland.
I Hajdas
Affiliation:
Paul Scherrer Institut (PSI), c/o Institute for Particle Physics, ETH Hönggerberg, CH-8093 Zürich, Switzerland.
*
Corresponding author. Email: heinz.gaeggeler@iac.unibe.ch.
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Abstract

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Radiocarbon enables a distinction between contemporary and fossil carbon, which can be used for the apportionment of biogenic and anthropogenic sources in environmental studies. In order to apply this approach to carbonaceous atmospheric aerosols, it is necessary to adapt pretreatment procedures to the requirements of 14C measurements. In this work, we followed an approach in which total carbon (TC) is subdivided into fractions of different chemical and physical properties. 14C data of ambient aerosols from Zürich (Switzerland) are presented for the 2 sub-fractions of TC, organic carbon (OC) and elemental carbon (EC). Furthermore, OC is separated into water-insoluble OC (WINSOC) and water-soluble OC (WSOC). Results demonstrate the importance to differentiate between these fractions for 14C-deduced source apportionment, as the contributions can range between both extremes, nearly exclusively biogenic and anthropogenic.

Type
Articles
Information
Radiocarbon , Volume 46 , Issue 1: Proceedings of the 18th International Radiocarbon Conference (Part 1 of 2), Conference Editors: Nancy Beavan Athfield, Rodger J Sparks , 2004 , pp. 475 - 484
Copyright
Copyright © 2004 by the Arizona Board of Regents on behalf of the University of Arizona 

References

Andreae, MO. 1983. Soot carbon and excess fine potassium: long-range transport of combustion-derived aerosols. Science 220:1148–51.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, doi: 10.1029/2001JD000574.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
Currie, LA, Eglinton, TI, Benner, BA Jr, Pearson, A. 1997. Radiocarbon “dating” of individual chemical compounds in atmospheric aerosol: first results comparing direct isotopic and multivariate statistical apportionment of specific polycyclic aromatic hydrocarbons. Nuclear Instruments and Methods in Physics Research B 123:475–86.Google Scholar
Currie, LA. 2000. Evolution and multidisciplinary frontiers of 14C aerosol science. Radiocarbon 42(1):115–26.Google Scholar
Currie, LA, Benner, BA Jr, Kessler, JD, Klinedinst, DB, Klouda, GA, Marolf, JV, Slater, JF, Wise, SA, Cachier, H, Cary, R, Chow, JC, Watson, J, Druffel, ERM, Masiello, CA, Eglinton, TI, Pearson, A, Reddy, CM, Gustafsson, Ö, Quinn, JG, Hartmann, PC, Hedges, JI, Prentice, KM, Kirchstetter, TW, Novakov, T, Puxbaum, H, Schmid, H. 2002. A critical evaluation of interlaboratory data on total, elemental, and isotopic carbon in the carbonaceous particle reference material, NIST SRM 1694a. Journal of Research of the National Institute of Standards and Technology 107:279–98.Google Scholar
Decesari, S, Facchini, MC, Matta, E, Lettini, F, Mircea, M, Fuzzi, S, Tagliavini, E, Putaud, J-P. 2001. Chemical features and seasonal variation of fine aerosol water-soluble organic compounds in the Po Valley, Italy. Atmospheric Environment 35:3691–9.Google Scholar
EMPA. 2000. Technischer Bericht zum Nationalen Beobachtungsnetz für Luftfremdstoffe (NABEL). Swiss Federal Laboratories for Materials Testing and Research (EMPA). Dübendorf, Switzerland.Google Scholar
Gelencsér, A, Hoffer, A, Molnár, A, Krivácsy, Z, Kiss, G, Mészáros, E. 2000. Thermal behaviour of carbonaceous aerosol from a continental background site. Atmospheric Environment 34:823–31.Google Scholar
ISO. 1995. Guide to the expression of uncertainty in measurement. International Organization for Standardization. Geneva, corrected and reprinted.Google Scholar
Jacobson, MC, Hansson, H-C, Noone, KJ, Charlson, RJ. 2000. Organic atmospheric aerosols: review and state of the science. Reviews of Geophysics 38:267–94.Google Scholar
Kalberer, M, Paulsen, D, Sax, M, Steinbacher, M, Dommen, J, Fisseha, R, Weingartner, E, Frankevich, V, Zenobi, R, Baltensperger, U. 2004. First identification of polymers as major components of atmospheric organic aerosols. Science 303:1659–62.Google Scholar
Keene, WC, Pszenny, AAP, Galloway, JN, Hawley, ME. 1986. Sea-salt corrections and interpretation of constituent ratios in marine precipitation. Journal of Geophysical Research 91:6647–58.Google Scholar
Kleefeld, S, Hoffer, A, Krivácsy, Z, Jennings, SG. 2002. Importance of organic and black carbon in atmospheric aerosols at Mace Head, on the west coast of Ireland (53$dG19'N, 9$dG54'W). Atmospheric Environment 36:4479–90.Google Scholar
Klinedinst, DB, Currie, LA. 1999. Direct quantification of PM2.5 fossil and biomass carbon within the Northern Front Range Air Quality Study's domain. Environmental Science and Technology 33:4146–54.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 35:6231–44.Google Scholar
Kubátová, A, Vermeylen, R, Claeys, M, Cafmeyer, J, Maenhaut, W. 2002. Organic compounds in urban aerosols from Gent, Belgium: characterization, sources, and seasonal differences. Journal of Geophysical Research 107:8343, doi: 10.1029/2001JD000556.Google Scholar
Lavanchy, VMH, Gäggeler, HW, Nyeki, S, Baltensperger, U. 1999. Elemental carbon (EC) and black carbon (BC) measurements with a thermal method and an aethalometer at the high-alpine research station Jungfraujoch. Atmospheric Environment 33:2759–69.CrossRefGoogle Scholar
Lemire, KR, Allen, DT, Klouda, GA, Lewis, CW. 2002. Fine particulate matter source attribution for southeast Texas using 14C/13C ratios. Journal of Geophysical Research 107:4613, doi: 10.1029/2002JD002339.Google Scholar
Levin, I, Kromer, B. 1997. Twenty years of atmospheric 14CO2 observations at Schauinsland station, Germany. Radiocarbon 39(2):205–18.Google Scholar
Levin, I, Kromer, B. 2002. Long-term measurements of 14CO2 at Jungfraujoch: observing fossil fuel CO2 over Europe. In: Workshop on “Atmospheric research at the Jungfraujoch and in the Alps,” Davos, Switzerland, 20 September 2002 (available at: http://acp.web.psi.ch/acp_public/ProceedingDavos02.pdf). p 19–20.Google Scholar
Matsumoto, K, Kawamura, K, Uchida, M, Shibata, Y, Yoneda, M. 2001. Compound specific radiocarbon and δ13C measurements of fatty acids in a continental aerosol sample. Geophysical Research Letters 28: 4587–90.Google Scholar
NIST. 2001. Certificate of analysis for Standard Reference Material 1649a, Urban Dust. National Institute of Standards and Technology. Gaithersburg, Maryland, revised.Google Scholar
Pun, BK, Seigneur, C, Grosjean, D, Saxena, P. 2000. Gas-phase formation of water-soluble organic compounds in the atmosphere: a retrosynthetic analysis. Journal of Atmospheric Chemistry 35:199–223.Google Scholar
Reddy, CM, Pearson, A, Xu, L, McNichol, AP, Benner, BA Jr., Wise, SA, Klouda, GA, Currie, LA, Eglinton, TI. 2002. Radiocarbon as a tool to apportion the sources of polycyclic aromatic hydrocarbons and black carbon in environmental samples. Environmental Science and Technology 36:1774–82.Google Scholar
Rogge, WF, Mazurek, MA, Hildemann, LM, Cass, GR, Simoneit, BRT. 1993. Quantification of urban organic aerosol at a molecular level: identification, abundance and seasonal variation. Atmospheric Environment 27A:1309–30.Google Scholar
Rudolph, J, Anderson, RS, Czapiewski, KV, Czuba, E, Ernst, D, Gillespie, T, Huang, L, Rigby, C, Thompson, AE. 2003. The stable carbon isotope ratio of biogenic emissions of isoprene and the potential use of stable isotope ratio measurements to study photochemical processing of isoprene in the atmosphere. Journal of Atmospheric Chemistry 44:39–55.Google Scholar
Saurer, M, Borella, S, Schweingruber, F, Siegwolf, R. 1997. Stable carbon isotopes in tree rings of beech: climatic versus site-related influences. Trees 11:291–7.Google Scholar
Schmid, H, Laskus, L, Abraham, HJ, Baltensperger, U, Lavanchy, V, Bizjak, M, Burba, P, Cachier, H, Crow, D, Chow, J, Gnauk, T, Even, A, ten Brink, HM, Giesen, K-P, Hitzenberger, R, Hueglin, C, Maenhaut, W, Pio, C, Carvalho, A, Putaud, J-P, Toom-Sauntry, D, Puxbaum, H. 2001. Results of the “Carbon Conference” international aerosol carbon round robin test stage I. Atmospheric Environment 35:2111–21.Google Scholar
Schwikowski, M, Döscher, A, Gäggeler, HW, Schotterer, U. 1999. Anthropogenic versus natural sources of atmospheric sulphate from an Alpine ice core. Tellus 51B:938–51.Google Scholar
Slater, JF, Currie, LA, Dibb, JE, Benner, BA Jr. 2002. Distinguishing the relative contribution of fossil fuel and biomass combustion aerosols deposited at Summit, Greenland through isotopic and molecular characterization of insoluble carbon. Atmospheric Environment 36:4463–77.CrossRefGoogle Scholar
Synal, H-A, Jacob, S, Suter, M. 2000. The PSI/ETH small radiocarbon dating system. Nuclear Instruments and Methods in Physics Research B 172:1–7.CrossRefGoogle Scholar
Szidat, S, Jenk, TM, Gäggeler, HW, Synal, H-A, Hajdas, I, Bonani, G, Saurer, M. 2004a. THEODORE, a two-step heating system for the EC/OC determination of radiocarbon (14C) in the environment. Nuclear Instruments and Methods in Physics Research B , in press.CrossRefGoogle Scholar
Szidat, S, Jenk, TM, Gäggeler, HW, Synal, H-A, Fisseha, R, Baltensperger, U, Kalberer, M, Samburova, V, Reimann, S, Hajdas, I. 2004b. Radiocarbon (14C) deduced biogenic and anthropogenic contributions to organic carbon (OC) of urban aerosols from Zürich, Switzerland. Atmospheric Environment , in press.Google Scholar
Turpin, BJ, Saxena, P, Andrews, E. 2000. Measuring and simulating particulate organics in the atmosphere: problems and prospects. Atmospheric Environment 34:2983–3013.Google Scholar
Zheng, M, Wan, TSM, Fang, M, Wang, F. 1997. Characterization of the non-volatile organic compounds in the aerosols of Hong Kong—identification, abundance and origin. Atmospheric Environment 31:227–37.Google Scholar