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A Preparative 2D-Chromatography Method for Compound-Specific Radiocarbon Analysis of Dicarboxylic Acids in Aerosols

Published online by Cambridge University Press:  18 July 2016

S M Fahrni
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Bern, Switzerland Paul Scherrer Institut, Villigen, Switzerland Oeschger Centre for Climate Change Research, University of Bern, Bern, Switzerland
M Ruff
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Bern, Switzerland Paul Scherrer Institut, Villigen, Switzerland Ion Beam Physics, ETH Hönggerberg, Zurich, Switzerland
L Wacker
Affiliation:
Ion Beam Physics, ETH Hönggerberg, Zurich, Switzerland
N Perron
Affiliation:
Paul Scherrer Institut, Villigen, Switzerland
H W Gäggeler
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Bern, Switzerland Paul Scherrer Institut, Villigen, Switzerland
S Szidat*
Affiliation:
Department of Chemistry and Biochemistry, University of Bern, Bern, Switzerland Oeschger Centre for Climate Change Research, University of Bern, Bern, Switzerland
*
Corresponding author. Email: [email protected]
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Abstract

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There is a great scientific demand for an assessment of the sources and formation processes of atmospheric carbonaceous aerosols since they strongly influence the global radiation balance and affect public health. Much attention in atmospheric studies has been paid to dicarboxylic acids (DCAs) due to their abundance at substantially different sites and their potential influence on cloud formation processes. Nevertheless, sources of oxalic acid (HOOCCOOH) and other DCAs are not well understood yet. In order to quantify contributions of fossil and non-fossil sources, a method for the preparative separation of oxalic acid and other DCAs from aerosols for compound-specific radiocarbon analysis (CSRA) has been developed. This method consists of a water extraction of aerosols collected on quartz-fiber filters followed by 2 consecutive liquid chromatography (LC) steps on different chromatography columns (2D-chromatography). Through the use of aqueous, completely non-organic eluents and single injections into liquid chromatography, low blank levels are achieved with total oxalic acid recoveries of up to 66%. Upon separation, 14C measurements of small samples (containing typically 10–20 μg carbon) are conducted at the gas ion source of the 200kV accelerator mass spectrometry facility MICADAS. The method is verified with processed reference materials, artificial mixtures of oxalic acid with typical matrix components, and a standard addition of ambient aerosols. Two exemplary field samples show dominant non-fossil sources of oxalic acid.

Type
Methods, Applications, and Developments
Copyright
Copyright © 2010 by the Arizona Board of Regents on behalf of the University of Arizona 

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