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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Preprints
https://doi.org/10.5194/amt-2020-221
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-2020-221
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  15 Jul 2020

15 Jul 2020

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A revised version of this preprint was accepted for the journal AMT and is expected to appear here in due course.

Interferences on Aerosol Acidity Quantification due to Gas-phase Ammonia Uptake onto Acidic Sulfate Filter Samples

Benjamin A. Nault1,2, Pedro Campuzano-Jost1,2, Douglas A. Day1,2, Hongyu Guo1,2, Duesong S. Jo1,2,a, Anne V. Handscy1,2, Demetrios Pagonis1,2, Jason C. Schroder1,2,b, Melinda K. Schueneman1,2, Michael J. Cubison3, Jack E. Dibb4, Alma Hodzic5, Weiwei Hu6, Brett B. Palm7, and Jose L. Jimenez1,2 Benjamin A. Nault et al.
  • 1Department of Chemistry, University of Colorado, Boulder, CO, USA
  • 2Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 3TOFWERK AG, Boulder, CO, USA
  • 4Earth Systems Research Center, Institute for the Study of Earth, Oceans, and Space, University of New Hampshire, Durham, NH, USA
  • 5Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
  • 6State Key Laboratory at Organic Geochemistry, Guangzhou, Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, China
  • 7Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
  • anow at: Advanced Study Program, National Center for Atmospheric Research, Boulder, CO, USA
  • bnow at: Colorado Department of Public Health and Environment, Denver, CO, USA

Abstract. Measurements of the mass concentration and chemical speciation of aerosols are important to investigate their chemical and physical processing from near emission sources to the most remote regions of the atmosphere. A common method to analyze aerosols is to collect them onto filters and to analyze filters off-line; however, biases in some chemical components are possible due to changes in the accumulated particles during the handling of the samples. Any biases would impact the measured chemical composition, which in turn affects our understanding of numerous physico-chemical processes and aerosol radiative properties. We show, using filters collected onboard the NASA DC-8 and NSF C-130 during six different aircraft campaigns, a consistent, substantial difference in ammonium mass concentration and ammonium-to-anion ratios, when comparing the aerosols collected on filters versus the Aerodyne Aerosol Mass Spectrometer (AMS). Another on-line measurement is consistent with the AMS in showing that the aerosol has lower ammonium-to-anion ratios than obtained by the filters. Using a gas uptake model with literature values for accommodation coefficients, we show that for ambient ammonia mixing ratios greater than 10 ppbv, the time scale for ammonia reacting with acidic aerosol on filter substrates is less than 30 s (typical filter handling time in the aircraft) for typical aerosol volume distributions. Measurements of gas-phase ammonia inside the cabin of the DC-8 show ammonia mixing ratios of 45 ± 20 ppbv, consistent with mixing ratios observed in other indoor environments. This analysis enables guidelines for filter handling to reduce ammonia uptake. Finally, a more meaningful limit-of-detection for filters that either do not have an ammonia scrubber and/or are handled in the presence of human emissions is ∼0.2 μg m−3 ammonium, which is substantially higher than the limit-of-detection of the ion chromatography.

Benjamin A. Nault et al.

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Benjamin A. Nault et al.

Data sets

ATom: Merged Atmospheric Chemistry, Trace Gases, and Aerosols S.C. Wofsy, S. Afshar, H.M. Allen, E.C. Apel, E.C. Asher, B. Barletta, J. Bent, H. Bian, B.C. Biggs, D.R. Blake, N. Blake, I. Bourgeois, C.A. Brock, W.H. Brune, J.W. Budney, T.P. Bui, A. Butler, P. Campuzano-Jost, C.S. Chang, M. Chin, R. Commane, G. Correa, J.D. Crounse, P. D. Cullis, B.C. Daube, D.A. Day, J.M. Dean-Day, J.E. Dibb, J.P. DiGangi, G.S. Diskin, M. Dollner, J.W. Elkins, F. Erdesz, A.M. Fiore, C.M. Flynn, K.D. Froyd, D.W. Gesler, S.R. Hall, T.F. Hanisco, R.A. Hannun, A.J. Hills, E.J. Hintsa, A. Hoffman, R.S. Hornbrook, L.G. Huey, S. Hughes, J.L. Jimenez, B.J. Johnson, J.M. Katich, R.F. Keeling, M.J. Kim, A. Kupc, L.R. Lait, J.-F. Lamarque, J. Liu, K. McKain, R.J. Mclaughlin, S. Meinardi, D.O. Miller, S.A. Montzka, F.L. Moore, E.J. Morgan, D.M. Murphy, L.T. Murray, B.A. Nault, J.A. Neuman, P.A. Newman, J.M. Nicely, X. Pan, W. Paplawsky, J. Peischl, M.J. Prather, D.J. Price, E. Ray, J.M. Reeves, M. Richardson, A.W. Rollins, K.H. Rosenlof, T.B. Ryerson, E. Scheuer, G.P. Schill, J.C. Schroder, J.P. Schwarz, J.M. St.Clair, S.D. Steenrod, B.B. Stephens, S.A. Strode, C. Sweeney, D. Tanner, A.P. Teng, A.B. Thames, C.R. Thompson, K. Ullmann, P.R. Veres, N. Vieznor, N.L. Wagner, A. Watt, R. Weber, B. Weinzierl, P.O. Wennberg, C.J. Williamson, J.C. Wilson, G.M. Wolfe, C.T. Woods, and L.H. Zeng https://doi.org/10.3334/ORNLDAAC/1581

ARCTAS-A and -B Merged SAGA Time Based Data A. Aknan, G. Chen, B. Anderson, E. Apel, D Blake, W. Brune, C. Cantrell, R. Cohen, J. Dibb, G. Diskin, A. Fried, J. Hair, G. Huey, J. L. Jimenez, Y. Kondo, L. Mauldin, A. Nenes, R. Shetter, R. Talbot, S. Vay, R. Weber, A. Weinheimer, P. Wennberg, A. Wisthaler https://doi.org/10.5067/SUBORBITAL/ARCTAS2008/DATA001

SEAC4RS Data A. Aknan, G. Chen, B. Anderson, A. Beyersdorf, D. Blake, C. Brock, A. Bucholtz, P. Bui, R. Cohen, A. DaSilva, J. Dibb, G. Diskin, A. Fried, K. Froyd, R.S. Gao, J. Hair, S. Hall, T. Hanisco, G. Huey, J. L. Jimenez, D. Lack, P. Lawson, V. Martins, P. Minnis, A. Nenes, P. Russell, T. Ryerson, S. Schmidt, A. Sorooshian, S. Tanelli, D. Vangilst, N. Wagner, R. Weber, P. Wennberg, A. Wisthaler https://doi.org/10.5067/Aircraft/SEAC4RS/Aerosol-TraceGas-Cloud

Benjamin A. Nault et al.

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Short summary
Collecting particulate matter, or aerosols, onto filters to be analyzed off-line is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Collecting particulate matter, or aerosols, onto filters to be analyzed off-line is a widely...
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