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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Volume 11, issue 5 | Copyright
Atmos. Meas. Tech., 11, 2749-2768, 2018
https://doi.org/10.5194/amt-11-2749-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 14 May 2018

Research article | 14 May 2018

Characterization of a catalyst-based conversion technique to measure total particulate nitrogen and organic carbon and comparison to a particle mass measurement instrument

Chelsea E. Stockwell1,2, Agnieszka Kupc1,2, Bartłomiej Witkowski1,2,3, Ranajit K. Talukdar1,2, Yong Liu4, Vanessa Selimovic5, Kyle J. Zarzana1,2, Kanako Sekimoto1,2, Carsten Warneke1,2, Rebecca A. Washenfelder1, Robert J. Yokelson5, Ann M. Middlebrook1, and James M. Roberts1 Chelsea E. Stockwell et al.
  • 1NOAA Earth System Research Laboratory (ESRL), Chemical Sciences Division, Boulder, CO 80305, USA
  • 2Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
  • 3Faculty of Chemistry, University of Warsaw, al. Żwirki i Wigury 101, 02-089, Warsaw, Poland
  • 4Department of Chemistry, University of Colorado Denver, Denver, CO 80217, USA
  • 5Department of Chemistry, University of Montana, Missoula, MT 59812, USA

Abstract. The chemical composition of aerosol particles is a key aspect in determining their impact on the environment. For example, nitrogen-containing particles impact atmospheric chemistry, air quality, and ecological N deposition. Instruments that measure total reactive nitrogen (Nr = all nitrogen compounds except for N2 and N2O) focus on gas-phase nitrogen and very few studies directly discuss the instrument capacity to measure the mass of Nr-containing particles. Here, we investigate the mass quantification of particle-bound nitrogen using a custom Nr system that involves total conversion to nitric oxide (NO) across platinum and molybdenum catalysts followed by NO−O3 chemiluminescence detection. We evaluate the particle conversion of the Nr instrument by comparing to mass-derived concentrations of size-selected and counted ammonium sulfate ((NH4)2SO4), ammonium nitrate (NH4NO3), ammonium chloride (NH4Cl), sodium nitrate (NaNO3), and ammonium oxalate ((NH4)2C2O4) particles determined using instruments that measure particle number and size. These measurements demonstrate Nr-particle conversion across the Nr catalysts that is independent of particle size with 98±10% efficiency for 100–600nm particle diameters. We also show efficient conversion of particle-phase organic carbon species to CO2 across the instrument's platinum catalyst followed by a nondispersive infrared (NDIR) CO2 detector. However, the application of this method to the atmosphere presents a challenge due to the small signal above background at high ambient levels of common gas-phase carbon compounds (e.g., CO2). We show the Nr system is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation using single-component, laboratory-generated, Nr-containing particles below 2.5µm in size. In addition we show agreement with mass measurements of an independently calibrated online particle-into-liquid sampler directly coupled to the electrospray ionization source of a quadrupole mass spectrometer (PILS–ESI/MS) sampling in the negative-ion mode. We obtain excellent correlations (R2= 0.99) of particle mass measured as Nr with PILS–ESI/MS measurements converted to the corresponding particle anion mass (e.g., nitrate, sulfate, and chloride). The Nr and PILS–ESI/MS are shown to agree to within ∼6% for particle mass loadings of up to 120µgm−3. Consideration of all the sources of error in the PILS–ESI/MS technique yields an overall uncertainty of ±20% for these single-component particle streams. These results demonstrate the Nr system is a reliable direct particle mass measurement technique that differs from other particle instrument calibration techniques that rely on knowledge of particle size, shape, density, and refractive index.

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This work investigates the total conversion of particle-bound nitrogen and organic carbon across platinum and molybdenum catalysts followed by NO–O3 chemiluminescence and nondispersive infrared CO2 detection. We show the instrument is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation through comparisons with a calibrated particle-into-liquid sampler coupled to an electrospray ionization source of a mass spectrometer.
This work investigates the total conversion of particle-bound nitrogen and organic carbon across...
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