Hostname: page-component-848d4c4894-pftt2 Total loading time: 0 Render date: 2024-05-25T08:14:16.927Z Has data issue: false hasContentIssue false

Microgram-Level Radiocarbon Determination of Carbonaceous Particles in Firn and Ice Samples: Pretreatment and OC/EC Separation

Published online by Cambridge University Press:  09 February 2016

Fang Cao
Affiliation:
Paul Scherrer Institute, Villigen, Switzerland Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, China
Yan-Lin Zhang
Affiliation:
Paul Scherrer Institute, Villigen, Switzerland Oeschger Centre for Climate Change Research, University of Bern, Switzerland Department of Chemistry and Biochemistry, University of Bern, Switzerland
Sönke Szidat
Affiliation:
Oeschger Centre for Climate Change Research, University of Bern, Switzerland Department of Chemistry and Biochemistry, University of Bern, Switzerland
Alexander Zapf
Affiliation:
Paul Scherrer Institute, Villigen, Switzerland Oeschger Centre for Climate Change Research, University of Bern, Switzerland
Lukas Wacker
Affiliation:
Laboratory of Ion Beam Physics, ETH, Zurich, Switzerland
Margit Schwikowski*
Affiliation:
Paul Scherrer Institute, Villigen, Switzerland Oeschger Centre for Climate Change Research, University of Bern, Switzerland Department of Chemistry and Biochemistry, University of Bern, Switzerland
*
6Corresponding author. Email: margit.schwikowski@psi.ch.

Abstract

Carbonaceous particles that comprise organic carbon (OC) and elemental carbon (EC) are of increasing interest in climate research because of their influence on the radiation balance of the Earth. The radiocarbon determination of particulate OC and EC extracted from ice cores provides a powerful tool to reconstruct the long-term natural and anthropogenic emissions of carbonaceous particles. However, this 14C-based source apportionment method has not been applied for the firn section, which is the uppermost part of Alpine glaciers with a typical thickness of up to 50 m. In contrast to glacier ice, firn samples are more easily contaminated through drilling and handling operations. In this study, an alternative decontamination method for firn samples consisting of chiselling off the outer parts instead of rinsing them was developed and verified. The obtained procedural blank of 2.8 ± 0.8 μg C for OC is a factor of 2 higher compared to the rinsing method used for ice, but still relatively low compared to the typical OC concentration in firn samples from Alpine glaciers. The EC blank of 0.3 ± 0.1 μg C is similar for both methods. For separation of OC and EC for subsequent 14C analysis, a thermal-optical method instead of the purely thermal method was applied for the first time to firn and ice samples, resulting in a reduced uncertainty of both the mass and 14C determination. OC and EC concentrations as well as their corresponding fraction of modern for firn and ice samples from Fiescherhorn and Jungfraujoch agree well with published results, validating the new method.

Type
Articles
Copyright
Copyright © 2013 by the Arizona Board of Regents on behalf of the University of Arizona 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

Footnotes

Deceased.

References

Bukowiecki, N, Zieger, P, Weingartner, E, Juranyi, Z, Gysel, M, Neininger, B, Schneider, B, Hueglin, C, Ulrich, A, Wichser, A, Henne, S, Brunner, D, Kaegi, R, Schwikowski, M, Tobler, L, Wienhold, FG, Engel, I, Buchmann, B, Peter, T, Baltensperger, U. 2011. Ground-based and airborne in-situ measurements of the Eyjafjallajökull volcanic aerosol plume in Switzerland in spring 2010. Atmospheric Chemistry and Physics 11:10,01130.Google Scholar
Currie, LA. 2000. Evolution and multidisciplinary frontiers of 14C aerosol science. Radiocarbon 42(1):115–26.Google Scholar
Fahrni, SM, Wacker, L, Synal, HA, Szidat, S. 2013. Improving a gas ion source for 14C AMS. Nuclear Instruments and Methods in Physics Research B 294:320–7.Google Scholar
Intergovernmental Panel on Climate Change (IPCC). 2007. Climate Change 2007: The Physical Science Basis: Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change. Solomon, S, Qin, D, Manning, M, Chen, Z, Marquis, M, Averyt, KB, Tignor, M, editors. Cambridge: Cambridge University Press.Google Scholar
Jenk, TM, Szidat, S, Schwikowski, M, Gäggeler, HW, Brütsch, S, Wacker, L, Synal, H-A, Saurer, M. 2006. Radiocarbon analysis in an Alpine ice core: record of anthropogenic and biogenic contributions to carbonaceous aerosols in the past (1650–1940). Atmospheric Chemistry and Physics 6:5381–90.Google Scholar
Jenk, TM, Szidat, S, Schwikowski, M, Gäggeler, HW, Wacker, L, Synal, H-A, Saurer, M. 2007. Microgram level radiocarbon (14C) determination on carbonaceous particles in ice. Nuclear Instruments and Methods in Physics Research B 259(1):518–25.Google Scholar
Legrand, M, Preunkert, S, Schock, M, Cerqueira, M, Kasper-Giebl, A, Afonso, J, Pio, C, Gelencsér, A, Dombrowski-Etchevers, I. 2007. Major 20th century changes of carbonaceous aerosol components (EC, WinOC, DOC, HULIS, carboxylic acids, and cellulose) derived from Alpine ice cores. Journal of Geophysical Research 112: D23S11, doi:10.1029/2006JD008080.Google Scholar
May, B, Wagenbach, D, Hammer, S, Steier, P, Puxbaum, H, Pio, C. 2009. The anthropogenic influence on carbonaceous aerosol in the European background. Tellus B 61(2):464–72.Google Scholar
Minguillón, MC, Perron, N, Querol, X, Szidat, S, Fahrni, SM, Alastuey, A, Jimenez, JL, Mohr, C, Ortega, AM, Day, DA, Lanz, VA, Wacker, L, Reche, C, Cusack, M, Amato, F, Kiss, G, Hoffer, A, Decesari, S, Moretti, F, Hillamo, R, Teinilä, K, Seco, R, Peñuelas, J, Metzger, A, Schallhart, S, Müller, M, Hansel, A, Burkhart, JF, Baltensperger, U, Prévôt, ASH. 2011. Fossil versus contemporary sources of fine elemental and organic carbonaceous particulate matter during the DAURE campaign in Northeast Spain. Atmospheric Chemistry and Physics 11:12,06784.Google Scholar
Pöschl, U. 2005. Atmospheric aerosols: composition, transformation, climate and health effects. Angewandte Chemie International Edition 44(46):7520–40.Google Scholar
Ruff, M, Wacker, L, Gäggeler, HW, Suter, M, Synal, H-A, Szidat, S. 2007. A gas ion source for radiocarbon measurements at 200 kV. Radiocarbon 49(2):307–14.Google Scholar
Ruff, M, Fahrni, S, Gäggeler, HW, Hajdas, I, Suter, M, Synal, H-A, Szidat, S, Wacker, L. 2010. On-line radiocarbon measurements of small samples using elemental analyzer and MICADAS gas ion source. Radiocarbon 52(4):1645–56.Google Scholar
Sigl, M, Jenk, TM, Kellerhals, T, Szidat, S, Gäggeler, HW, Wacker, L, Synal, H-A, Boutron, C, Barbante, C, Gabrieli, J, Schwikowski, M. 2009. Towards radiocarbon dating of ice cores. Journal of Glaciology 55(194):985–96.Google Scholar
Steier, P, Drosg, R, Fedi, M, Kutschera, W, Schock, M, Wagenbach, D, Wild, EM. 2006. Radiocarbon determination of particulate organic carbon in non-temperated, Alpine glacier ice. Radiocarbon 48(1):6982.Google Scholar
Stuiver, M, Polach, HA. 1977. Discussion: reporting of 14C data. Radiocarbon 19(3):355–63.Google Scholar
Synal, H-A, Stocker, M, Suter, M. 2007. MICADAS: a new compact radiocarbon AMS system. Nuclear Instruments and Methods in Physics Research B 259(1):713.Google Scholar
Szidat, S, Jenk, TM, Gäggeler, HW, Synal, H-A, Fisseha, R, Baltensperger, U, Kalberer, M, Samburova, V, Reimann, S, Kasper-Giebl, A, Hajdas, I. 2004a. Radiocarbon (14C)-deduced biogenic and anthropogenic contributions to organic carbon (OC) of urban aerosols from Zürich, Switzerland. Atmospheric Environment 38(24):4035–44.Google Scholar
Szidat, S, Jenk, TM, Gäggeler, HW, Synal, H-A, Hajdas, I, Bonani, G, Saurer, M. 2004b. 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 223–224:829–36.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(D7):D07206, doi:10.1029/2005JD006590.Google Scholar
Szidat, S, Ruff, M, Perron, N, Wacker, L, Synal, H-A, 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 Goeteborg, Sweden. Atmospheric Chemistry and Physics 9:1521–35.Google Scholar
Szidat, S, Bench, G, Bernardoni, V, Calzolai, G, Czimczik, CI, Derendorp, L, Dusek, U, Elder, K, Fedi, M, Genberg, J, Gustafsson, Ö, Kirillova, E, Kondo, M, McNichol, AP, Perron, N, Santos, GM, Stenström, K, Swietlicki, E, Ushida, M, Wacker, L, Vecchi, R, Zhang, YL, Prévôt, ASH. 2013. Intercomparison of 14C analysis of carbonaceous aerosols: Exercise 2009. Radiocarbon, these proceedings, doi:10.2458/azu_js_rc.55.16314.Google Scholar
Wacker, L, Fahrni, SM, Hajdas, I, Molnár, M, Synal, H-A, Szidat, S, Zhang, YL. 2013. A versatile gas interface for routine radiocarbon analysis with a gas ion source. Nuclear Instruments and Methods in Physics Research B 294:315–9.Google Scholar
Zhang, YL, Liu, D, Shen, CD, Ding, P, Zhang, G. 2010. Development of a preparation system for the radiocarbon analysis of organic carbon in carbonaceous aerosols in China. Nuclear Instruments and Methods in Physics Research B 268(17–18):2831–4.Google Scholar
Zhang, YL, Perron, N, Ciobanu, VG, Zotter, P, Minguillón, MC, Wacker, L, Prévôt, ASH, Baltensperger, U, Szidat, S. 2012. On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols. Atmospheric Chemistry and Physics 12:10,84156.Google Scholar
Zhang, YL, Zotter, P, Perron, N, Prévôt, ASH, Wacker, L, Szidat, S. 2013. Fossil and non-fossil sources of different carbonaceous fractions in fine and coarse particles by radiocarbon measurement. Radiocarbon, these proceedings, doi:10.2458/azu_js_rc.55.16278.Google Scholar