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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union

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https://doi.org/10.5194/amt-2017-442
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article
02 May 2018
Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Measurement Techniques (AMT).
Field measurements of methylglyoxal using Proton Transfer Reaction-Time of Flight Mass Spectrometry and comparison to the DNPH/HPLC-UV method
Vincent Michoud1,2, Stéphane Sauvage1, Thierry Léonardis1, Isabelle Fronval1, Alexandre Kukui3, Nadine Locoge1, and Sébastien Dusanter1 1IMT Lille Douai, Univ. Lille, SAGE – Département Sciences de l'Atmosphère et Génie de l'Environnement, 59000 Lille, France
2LISA/IPSL, Laboratoire Interuniversitaire des Systèmes Atmosphériques, UMR CNRS 7583, Université Paris Est Créteil (UPEC) et Université Paris Diderot (UPD), Créteil, France
3Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), UMR6115 CNRS – Université d'Orléans, 45071 Orléans CEDEX 2, France
Abstract. Methylglyoxal (MGLY) is an important atmospheric α-dicarbonyl species whose photolysis acts as a significant source of peroxy radicals, contributing to the oxidizing capacity of the atmosphere and, as such, the formation of secondary pollutants such as organic aerosols and ozone. However, despite its importance, only a few techniques exhibit time resolutions and detection limits that are suitable for atmospheric measurements.

This study present, to the best of our knowledge, the first measurements of ambient MGLY using Proton Transfer Reaction-Time of Flight Mass Spectrometry (PTR-ToFMS). These measurements were performed during the ChArMEx SOP2 field campaign. This campaign took place at a Mediterranean site characterized by intense biogenic emissions and low levels of anthropogenic trace gases. Concomitant measurements of MGLY were performed using the 2,4-dinitrophenylhydrazine (DNPH) derivatization technique and High Performance Liquide Chromatography (HPLC) with UV detection. PTR-ToFMS and DNPH-HPLC measurements were compared to determine whether these techniques can perform reliable measurements of MGLY.

Ambient time series revealed levels of MGLY ranging from 28–365 pptv, with a clear diurnal cycle due to elevated concentrations of primary biogenic species during daytime, whose oxidation led to large production rates of MGLY. A scatter plot of the PTR-ToFMS and DNPH-HPLC measurements indicates a reasonable correlation (R2 = 0.48) but a slope significantly lower than unity (0.58 ± 0.05) and a significant intercept of 88.3 ± 8.0 pptv. A careful investigation of the differences between the two techniques suggests that this disagreement is not due to spectrometric interferences from H3O+(H2O)3, MEK (or butanal) detected at m/z 73.050 and m/z 73.065, respectively, which are close to the MGLY m/z of 73.029. The differences are more likely due to uncorrected sampling artefacts such as overestimated collection efficiency or loss of MGLY into the sampling line for the DNPH-HPLC technique or unknown isobaric interfering compounds such as acrylic acid and propanediol for the PTR-ToFMS.

Calculations of MGLY loss rates with respect to OH-oxidation and direct photolysis indicate similar contributions for these two loss pathways.

Citation: Michoud, V., Sauvage, S., Léonardis, T., Fronval, I., Kukui, A., Locoge, N., and Dusanter, S.: Field measurements of methylglyoxal using Proton Transfer Reaction-Time of Flight Mass Spectrometry and comparison to the DNPH/HPLC-UV method, Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2017-442, in review, 2018.
Vincent Michoud et al.
Vincent Michoud et al.
Vincent Michoud et al.

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Short summary
This study present the first measurements of ambient methylglyoxal, an important atmospheric α-dicarbonyl, using Proton Transfer Reaction-Time of Flight Mass Spectrometry. These measurements fairly agree with concomitant measurements from a reference technic: DNPH derivatization technique and High Performance Liquide Chromatography with UV detection. In addition, a careful investigation of the differences between the two techniques is performed to explain the disagreements observed.
This study present the first measurements of ambient methylglyoxal, an important atmospheric...
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