Preprints
https://doi.org/10.5194/amt-2021-325
https://doi.org/10.5194/amt-2021-325

  29 Oct 2021

29 Oct 2021

Review status: this preprint is currently under review for the journal AMT.

High-Frequency Gaseous and Particulate Chemical Characterization using Extractive Electrospray Ionization Mass Spectrometry (Dual-Phase-EESI-TOF)

Chuan Ping Lee1, Mihnea Surdu1, David M. Bell1, Josef Dommen1, Mao Xiao1, Xueqin Zhou1, Andrea Baccarini1,2, Stamatios Giannoukos1,3, Günther Wehrle1, Pascal André Schneider1, Andre S. H. Prevot1, Jay G. Slowik1, Houssni Lamkaddam1, Dongyu Wang1, Urs Baltensperger1, and Imad El Haddad1 Chuan Ping Lee et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland
  • 2School of Architecture, Civil and Environmental Engineering, École Polytechnique Fédérale de Lausanne, Switzerland
  • 3Laboratory of Organic Chemistry, Department of Chemistry and Applied Bioscience, ETH Zurich, 8093 Zurich, Switzerland

Abstract. To elucidate the sources and chemical reaction pathways of organic vapors and particulate matter in the ambient atmosphere, real-time detection of both gas and particle phase is needed. State-of-the-art techniques often suffer from thermal decomposition, ionization-induced fragmentation, high cut-off size of aerosols or low time resolution. In response to all these limitations, we developed a new technique that uses extractive electrospray ionization (EESI) for online gas and particle chemical speciation, namely the dual-phase extractive electrospray ionization time-of-flight mass spectrometer (Dual-Phase-EESI-TOF or Dual-EESI in short). The Dual-EESI was designed and optimized to measure gas- and particle-phase species with saturation vapor concentrations spanning more than 10 orders of magnitude with good linearity and a measurement cycle as fast as 3 min. The gas-phase selectivity of the Dual-EESI was compared with that of nitrate chemical ionization mass spectrometry. In addition, we performed organic aerosol uptake experiments to characterize the relative gas and particle response factors. In general, the Dual-EESI is more sensitive toward gas-phase analytes as compared to their particle-phase counterparts. The real-time measurement capability of the Dual-EESI for chemically speciated gas- and particle-phase measurements can provide new insights into aerosol sources or formation mechanisms, where gas-particle partitioning behavior can be determined after absolute parameterization of the gas/particle sensitivity.

Chuan Ping Lee et al.

Status: open (extended)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on amt-2021-325', Anonymous Referee #2, 02 Dec 2021 reply

Chuan Ping Lee et al.

Chuan Ping Lee et al.

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Short summary
Real-time detection of both gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analytes.