Limited impact of sulfate-driven chemistry on black carbon aerosol aging in power plant plumes

Milos Z. Markovic; Anne E. Perring; Ru-Shan Gao; Jin Liao; Andre Welti; Nick L. Wagner; Ilana B. Pollack; Ann M. Middlebrook; Thomas B. Ryerson; Michael K. Trainer; Carsten Warneke; Joost A. de Gouw; David W. Fahey; Philip Stier; Joshua P. Schwarz; Milos Z. Markovic; Anne E. Perring; Ru-Shan Gao; Jin Liao; Andre Welti; Nick L. Wagner; Ilana B. Pollack; Ann M. Middlebrook; Thomas B. Ryerson; Michael K. Trainer; Carsten Warneke; Joost A. de Gouw; David W. Fahey; Philip Stier; Joshua P. Schwarz

doi:10.3934/environsci.2018.3.195

AIMS Environmental Science

2018, Volume 5, Issue 3: 195-215. doi: 10.3934/environsci.2018.3.195

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Research article

Limited impact of sulfate-driven chemistry on black carbon aerosol aging in power plant plumes

1.
Earth System Research Laboratory, Chemical Sciences Division, NOAA, Boulder, Colorado, USA
2.
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado, USA
3.
Department of Physics, University of Oxford, Oxford, Oxfordshire, United Kingdom
4.
Now at Picarro Inc, Santa Clara, CA, USA
5.
Now at Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, Maryland, and Universities Space Research Association, GESTAR, Columbia, Maryland
6.
Now at Finnish Meteorological Institute, Helsinki, Finland
7.
Now at Department of Atmospheric Science, Colorado State University, Ft. Collins, Colorado, USA

Received: 30 April 2018 Accepted: 18 June 2018 Published: 25 June 2018

The aging of refractory black carbon (rBC) aerosol by sulfate-driven chemistry has been constrained in coal-fired power-plant plumes using the NOAA WP-3D research aircraft during the Southern Nexus (SENEX) study, which took place in the Southeastern US in June and July of 2013. A Single Particle Soot Photometer (SP2) determined the microphysical properties of rBC-containing particles including single-particle rBC mass and the presence and amount of internally-mixed non-rBC material, hereafter referred to as “coatings”. Most power-plant influenced air was associated with very slightly increased amounts of non-refractory material, likely sulfate internally mixed with the rBC, however this increase was statistically insignificant even after semi-Lagrangian exposure for up to 5 h. On average, the increase in coating thickness was 2 ± 4 nm for particles containing 3–5 fg rBC. Similarly, the number fraction of rBC-containing particles that could be identified as internally mixed was increased by plume chemistry by only 1.3 ± 1.3%. These direct measurements of microphysical aging of rBC-containing aerosol by power plant emissions constrain the enhancement of sulfate chemistry on both rBC’s column-integrated absorption optical depth, and rBC-containing aerosol’s ability to act as cloud condensation nuclei. Appling Mie and k-Köhler theories to the SP2 observations, permits the resulting effect on rBC ambient light-absorption to be capped at the 2–6% level.
- black carbon aerosol,
- sulfate chemistry,
- aerosol aging,
- sulfate
Citation: Milos Z. Markovic, Anne E. Perring, Ru-Shan Gao, Jin Liao, Andre Welti, Nick L. Wagner, Ilana B. Pollack, Ann M. Middlebrook, Thomas B. Ryerson, Michael K. Trainer, Carsten Warneke, Joost A. de Gouw, David W. Fahey, Philip Stier, Joshua P. Schwarz. Limited impact of sulfate-driven chemistry on black carbon aerosol aging in power plant plumes[J]. AIMS Environmental Science, 2018, 5(3): 195-215. doi: 10.3934/environsci.2018.3.195

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Abstract

The aging of refractory black carbon (rBC) aerosol by sulfate-driven chemistry has been constrained in coal-fired power-plant plumes using the NOAA WP-3D research aircraft during the Southern Nexus (SENEX) study, which took place in the Southeastern US in June and July of 2013. A Single Particle Soot Photometer (SP2) determined the microphysical properties of rBC-containing particles including single-particle rBC mass and the presence and amount of internally-mixed non-rBC material, hereafter referred to as “coatings”. Most power-plant influenced air was associated with very slightly increased amounts of non-refractory material, likely sulfate internally mixed with the rBC, however this increase was statistically insignificant even after semi-Lagrangian exposure for up to 5 h. On average, the increase in coating thickness was 2 ± 4 nm for particles containing 3–5 fg rBC. Similarly, the number fraction of rBC-containing particles that could be identified as internally mixed was increased by plume chemistry by only 1.3 ± 1.3%. These direct measurements of microphysical aging of rBC-containing aerosol by power plant emissions constrain the enhancement of sulfate chemistry on both rBC’s column-integrated absorption optical depth, and rBC-containing aerosol’s ability to act as cloud condensation nuclei. Appling Mie and k-Köhler theories to the SP2 observations, permits the resulting effect on rBC ambient light-absorption to be capped at the 2–6% level.

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