Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

J. A. de Gouw; D. D. Parrish; S. S. Brown; Peter Edwards; J. B. Gilman; M. Graus; T. F. Hanisco; J. Kaiser; F. N. Keutsch; S. -W. Kim; B. M. Lerner; J. A. Neuman; J. B. Nowak; I. B. Pollack; J. M. Roberts; T. B. Ryerson; P. R. Veres; G. M. Wolfe

doi:10.1029/2019GL083044

Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

J. A. de Gouw, D. D. Parrish, S. S. Brown, Peter Edwards, J. B. Gilman, M. Graus, T. F. Hanisco, J. Kaiser, F. N. Keutsch, S. -W. Kim, B. M. Lerner, J. A. Neuman, J. B. Nowak, I. B. Pollack, J. M. Roberts, T. B. Ryerson, P. R. Veres, G. M. Wolfe

Chemistry

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Abstract

During an airborne study in the Southeast United States, measured mixing ratios of biogenic hydrocarbons were systematically lower in air masses containing enhanced nitrogen oxides from power plants, which we attribute to increased concentrations of hydroxyl (OH) radicals within the power plant plumes. Plume transects at successively further downwind distances provide a decreasing gradient of nitrogen oxides (NO _x) concentrations, which together with the implied loss rates of isoprene, constrains the OH dependence on NO _x. We find that OH concentrations were highest at nitrogen dioxide concentrations near 1–2 ppbv and decreased at higher and at lower concentrations. These findings agree with the dependence of OH on NO _x concentrations expected from known chemical reactions but are not consistent with some studies reporting direct OH measurements higher than expected in regions of the atmosphere with low NO _x (NO < 0.08 and NO ₂ < 0.46 ppbv) and high biogenic hydrocarbon emissions.

Original language	English
Pages (from-to)	7752-7760
Number of pages	9
Journal	Geophysical Research Letters
Volume	46
Issue number	13
Early online date	19 Jun 2019
DOIs	https://doi.org/10.1029/2019GL083044
Publication status	Published - 16 Jul 2019

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© 2019 American Geophysical Union. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

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10.1029/2019GL083044

Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of HydroxylRadicals
© 2019 American Geophysical Union. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.
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de Gouw, J. A., Parrish, D. D., Brown, S. S., Edwards, P., Gilman, J. B., Graus, M., Hanisco, T. F., Kaiser, J., Keutsch, F. N., Kim, S. .-W., Lerner, B. M., Neuman, J. A., Nowak, J. B., Pollack, I. B., Roberts, J. M., Ryerson, T. B., Veres, P. R., & Wolfe, G. M. (2019). Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals. Geophysical Research Letters, 46(13), 7752-7760. https://doi.org/10.1029/2019GL083044

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title = "Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals",

abstract = "During an airborne study in the Southeast United States, measured mixing ratios of biogenic hydrocarbons were systematically lower in air masses containing enhanced nitrogen oxides from power plants, which we attribute to increased concentrations of hydroxyl (OH) radicals within the power plant plumes. Plume transects at successively further downwind distances provide a decreasing gradient of nitrogen oxides (NO x) concentrations, which together with the implied loss rates of isoprene, constrains the OH dependence on NO x. We find that OH concentrations were highest at nitrogen dioxide concentrations near 1–2 ppbv and decreased at higher and at lower concentrations. These findings agree with the dependence of OH on NO x concentrations expected from known chemical reactions but are not consistent with some studies reporting direct OH measurements higher than expected in regions of the atmosphere with low NO x (NO < 0.08 and NO 2 < 0.46 ppbv) and high biogenic hydrocarbon emissions. ",

author = "{de Gouw}, {J. A.} and Parrish, {D. D.} and Brown, {S. S.} and Peter Edwards and Gilman, {J. B.} and M. Graus and Hanisco, {T. F.} and J. Kaiser and Keutsch, {F. N.} and Kim, {S. -W.} and Lerner, {B. M.} and Neuman, {J. A.} and Nowak, {J. B.} and Pollack, {I. B.} and Roberts, {J. M.} and Ryerson, {T. B.} and Veres, {P. R.} and Wolfe, {G. M.}",

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de Gouw, JA, Parrish, DD, Brown, SS, Edwards, P, Gilman, JB, Graus, M, Hanisco, TF, Kaiser, J, Keutsch, FN, Kim, S-W, Lerner, BM, Neuman, JA, Nowak, JB, Pollack, IB, Roberts, JM, Ryerson, TB, Veres, PR & Wolfe, GM 2019, 'Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals', Geophysical Research Letters, vol. 46, no. 13, pp. 7752-7760. https://doi.org/10.1029/2019GL083044

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T1 - Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

AU - de Gouw, J. A.

AU - Parrish, D. D.

AU - Brown, S. S.

AU - Edwards, Peter

AU - Gilman, J. B.

AU - Graus, M.

AU - Hanisco, T. F.

AU - Kaiser, J.

AU - Keutsch, F. N.

AU - Kim, S. -W.

AU - Lerner, B. M.

AU - Neuman, J. A.

AU - Nowak, J. B.

AU - Pollack, I. B.

AU - Roberts, J. M.

AU - Ryerson, T. B.

AU - Veres, P. R.

AU - Wolfe, G. M.

N1 - © 2019 American Geophysical Union. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

PY - 2019/7/16

Y1 - 2019/7/16

N2 - During an airborne study in the Southeast United States, measured mixing ratios of biogenic hydrocarbons were systematically lower in air masses containing enhanced nitrogen oxides from power plants, which we attribute to increased concentrations of hydroxyl (OH) radicals within the power plant plumes. Plume transects at successively further downwind distances provide a decreasing gradient of nitrogen oxides (NO x) concentrations, which together with the implied loss rates of isoprene, constrains the OH dependence on NO x. We find that OH concentrations were highest at nitrogen dioxide concentrations near 1–2 ppbv and decreased at higher and at lower concentrations. These findings agree with the dependence of OH on NO x concentrations expected from known chemical reactions but are not consistent with some studies reporting direct OH measurements higher than expected in regions of the atmosphere with low NO x (NO < 0.08 and NO 2 < 0.46 ppbv) and high biogenic hydrocarbon emissions.

AB - During an airborne study in the Southeast United States, measured mixing ratios of biogenic hydrocarbons were systematically lower in air masses containing enhanced nitrogen oxides from power plants, which we attribute to increased concentrations of hydroxyl (OH) radicals within the power plant plumes. Plume transects at successively further downwind distances provide a decreasing gradient of nitrogen oxides (NO x) concentrations, which together with the implied loss rates of isoprene, constrains the OH dependence on NO x. We find that OH concentrations were highest at nitrogen dioxide concentrations near 1–2 ppbv and decreased at higher and at lower concentrations. These findings agree with the dependence of OH on NO x concentrations expected from known chemical reactions but are not consistent with some studies reporting direct OH measurements higher than expected in regions of the atmosphere with low NO x (NO < 0.08 and NO 2 < 0.46 ppbv) and high biogenic hydrocarbon emissions.

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JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 13

ER -

Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

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