Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign

L. E. Gratz; J. L. Ambrose; D. A. Jaffe; C. Knote; L. Jaeglé; N. E. Selin; T. Campos; F. M. Flocke; M. Reeves; D. Stechman; M. Stell; A. J. Weinheimer; D. J. Knapp; D. D. Montzka; G. S. Tyndall; R. L. Mauldin; C. A. Cantrell; E. C. Apel; R. S. Hornbrook; N. J. Blake

doi:10.1016/j.atmosenv.2016.09.051

Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign

L. E. Gratz, J. L. Ambrose, D. A. Jaffe, C. Knote, L. Jaeglé, N. E. Selin, T. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, R. L. Mauldin, C. A. Cantrell, E. C. Apel, R. S. Hornbrook, N. J. Blake

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Abstract

Atmospheric emissions from the Chicago/Gary urban/industrial area significantly enhance ambient mercury (Hg) concentrations and lead to increased levels of atmospheric Hg deposition within the Lake Michigan Basin. We use airborne observations collected over Lake Michigan during the 2013 Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) campaign to quantify the outflow of total Hg (THg) emissions from the Chicago/Gary urban/industrial area. We use concurrent airborne measurements of THg, carbon monoxide (CO), nitrogen oxides (NO_x = NO + NO₂), and sulfur dioxide (SO₂) to calculate measured enhancement ratios and to characterize Chicago/Gary emissions with respect to the 2011 U.S. EPA National Emissions Inventory. We determine the observed THg/CO enhancement ratio in outflow from Chicago/Gary to be 0.21 ± 0.09 × 10⁻⁶ mol mol⁻¹ (ppqv/ppbv), which is comparable to observations reported for other major U.S. urban/industrial areas. We also employ the FLEXPART Lagrangian transport and dispersion model to simulate air mass transport during plume encounters and to compare our observations to inventoried emission ratios. We find that our observed THg/CO enhancement ratios are 63–67% greater than the transport-corrected emission ratios for the Chicago/Gary area. Our results suggest that there are many small emission sources that are not fully accounted for within the inventory, and/or that the re-emission of legacy Hg is a significant source of THg to the atmosphere in this region.

Original language	English
Pages (from-to)	415-423
Number of pages	9
Journal	Atmospheric Environment
Volume	145
DOIs	https://doi.org/10.1016/j.atmosenv.2016.09.051
State	Published - Nov 1 2016

Keywords

Airborne observations
Emission inventory
Enhancement ratio
Mercury
Urban area

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10.1016/j.atmosenv.2016.09.051

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Gratz, L. E., Ambrose, J. L., Jaffe, D. A., Knote, C., Jaeglé, L., Selin, N. E., Campos, T., Flocke, F. M., Reeves, M., Stechman, D., Stell, M., Weinheimer, A. J., Knapp, D. J., Montzka, D. D., Tyndall, G. S., Mauldin, R. L., Cantrell, C. A., Apel, E. C., Hornbrook, R. S., & Blake, N. J. (2016). Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign. Atmospheric Environment, 145, 415-423. https://doi.org/10.1016/j.atmosenv.2016.09.051

@article{78c4913c771d4acfbdc22c03ac6380d2,

title = "Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign",

abstract = "Atmospheric emissions from the Chicago/Gary urban/industrial area significantly enhance ambient mercury (Hg) concentrations and lead to increased levels of atmospheric Hg deposition within the Lake Michigan Basin. We use airborne observations collected over Lake Michigan during the 2013 Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) campaign to quantify the outflow of total Hg (THg) emissions from the Chicago/Gary urban/industrial area. We use concurrent airborne measurements of THg, carbon monoxide (CO), nitrogen oxides (NOx = NO + NO2), and sulfur dioxide (SO2) to calculate measured enhancement ratios and to characterize Chicago/Gary emissions with respect to the 2011 U.S. EPA National Emissions Inventory. We determine the observed THg/CO enhancement ratio in outflow from Chicago/Gary to be 0.21 ± 0.09 × 10−6 mol mol−1 (ppqv/ppbv), which is comparable to observations reported for other major U.S. urban/industrial areas. We also employ the FLEXPART Lagrangian transport and dispersion model to simulate air mass transport during plume encounters and to compare our observations to inventoried emission ratios. We find that our observed THg/CO enhancement ratios are 63–67\% greater than the transport-corrected emission ratios for the Chicago/Gary area. Our results suggest that there are many small emission sources that are not fully accounted for within the inventory, and/or that the re-emission of legacy Hg is a significant source of THg to the atmosphere in this region.",

keywords = "Airborne observations, Emission inventory, Enhancement ratio, Mercury, Urban area",

author = "Gratz, \{L. E.\} and Ambrose, \{J. L.\} and Jaffe, \{D. A.\} and C. Knote and L. Jaegl{\'e} and Selin, \{N. E.\} and T. Campos and Flocke, \{F. M.\} and M. Reeves and D. Stechman and M. Stell and Weinheimer, \{A. J.\} and Knapp, \{D. J.\} and Montzka, \{D. D.\} and Tyndall, \{G. S.\} and Mauldin, \{R. L.\} and Cantrell, \{C. A.\} and Apel, \{E. C.\} and Hornbrook, \{R. S.\} and Blake, \{N. J.\}",

note = "Publisher Copyright: {\textcopyright} 2016 Elsevier Ltd",

year = "2016",

month = nov,

day = "1",

doi = "10.1016/j.atmosenv.2016.09.051",

language = "English",

volume = "145",

pages = "415--423",

journal = "Atmospheric Environment",

issn = "1352-2310",

publisher = "Elsevier Ltd",

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Gratz, LE, Ambrose, JL, Jaffe, DA, Knote, C, Jaeglé, L, Selin, NE, Campos, T , Flocke, FM, Reeves, M, Stechman, D, Stell, M, Weinheimer, AJ, Knapp, DJ, Montzka, DD, Tyndall, GS, Mauldin, RL, Cantrell, CA, Apel, EC , Hornbrook, RS & Blake, NJ 2016, 'Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign', Atmospheric Environment, vol. 145, pp. 415-423. https://doi.org/10.1016/j.atmosenv.2016.09.051

TY - JOUR

T1 - Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign

AU - Gratz, L. E.

AU - Ambrose, J. L.

AU - Jaffe, D. A.

AU - Knote, C.

AU - Jaeglé, L.

AU - Selin, N. E.

AU - Campos, T.

AU - Flocke, F. M.

AU - Reeves, M.

AU - Stechman, D.

AU - Stell, M.

AU - Weinheimer, A. J.

AU - Knapp, D. J.

AU - Montzka, D. D.

AU - Tyndall, G. S.

AU - Mauldin, R. L.

AU - Cantrell, C. A.

AU - Apel, E. C.

AU - Hornbrook, R. S.

AU - Blake, N. J.

PY - 2016/11/1

Y1 - 2016/11/1

N2 - Atmospheric emissions from the Chicago/Gary urban/industrial area significantly enhance ambient mercury (Hg) concentrations and lead to increased levels of atmospheric Hg deposition within the Lake Michigan Basin. We use airborne observations collected over Lake Michigan during the 2013 Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) campaign to quantify the outflow of total Hg (THg) emissions from the Chicago/Gary urban/industrial area. We use concurrent airborne measurements of THg, carbon monoxide (CO), nitrogen oxides (NOx = NO + NO2), and sulfur dioxide (SO2) to calculate measured enhancement ratios and to characterize Chicago/Gary emissions with respect to the 2011 U.S. EPA National Emissions Inventory. We determine the observed THg/CO enhancement ratio in outflow from Chicago/Gary to be 0.21 ± 0.09 × 10−6 mol mol−1 (ppqv/ppbv), which is comparable to observations reported for other major U.S. urban/industrial areas. We also employ the FLEXPART Lagrangian transport and dispersion model to simulate air mass transport during plume encounters and to compare our observations to inventoried emission ratios. We find that our observed THg/CO enhancement ratios are 63–67% greater than the transport-corrected emission ratios for the Chicago/Gary area. Our results suggest that there are many small emission sources that are not fully accounted for within the inventory, and/or that the re-emission of legacy Hg is a significant source of THg to the atmosphere in this region.

AB - Atmospheric emissions from the Chicago/Gary urban/industrial area significantly enhance ambient mercury (Hg) concentrations and lead to increased levels of atmospheric Hg deposition within the Lake Michigan Basin. We use airborne observations collected over Lake Michigan during the 2013 Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) campaign to quantify the outflow of total Hg (THg) emissions from the Chicago/Gary urban/industrial area. We use concurrent airborne measurements of THg, carbon monoxide (CO), nitrogen oxides (NOx = NO + NO2), and sulfur dioxide (SO2) to calculate measured enhancement ratios and to characterize Chicago/Gary emissions with respect to the 2011 U.S. EPA National Emissions Inventory. We determine the observed THg/CO enhancement ratio in outflow from Chicago/Gary to be 0.21 ± 0.09 × 10−6 mol mol−1 (ppqv/ppbv), which is comparable to observations reported for other major U.S. urban/industrial areas. We also employ the FLEXPART Lagrangian transport and dispersion model to simulate air mass transport during plume encounters and to compare our observations to inventoried emission ratios. We find that our observed THg/CO enhancement ratios are 63–67% greater than the transport-corrected emission ratios for the Chicago/Gary area. Our results suggest that there are many small emission sources that are not fully accounted for within the inventory, and/or that the re-emission of legacy Hg is a significant source of THg to the atmosphere in this region.

KW - Airborne observations

KW - Emission inventory

KW - Enhancement ratio

KW - Mercury

KW - Urban area

UR - https://www.scopus.com/pages/publications/84989201353

U2 - 10.1016/j.atmosenv.2016.09.051

DO - 10.1016/j.atmosenv.2016.09.051

M3 - Article

AN - SCOPUS:84989201353

SN - 1352-2310

VL - 145

SP - 415

EP - 423

JO - Atmospheric Environment

JF - Atmospheric Environment

ER -

Airborne observations of mercury emissions from the Chicago/Gary urban/industrial area during the 2013 NOMADSS campaign

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Keywords

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