NOx Lifetime and NOy Partitioning During WINTER

Hannah S. Kenagy; Tamara L. Sparks; Carlena J. Ebben; Paul J. Wooldrige; Felipe D. Lopez-Hilfiker; Ben H. Lee; Joel A. Thornton; Erin E. McDuffie; Dorothy L. Fibiger; Steven S. Brown; Denise D. Montzka; Andrew J. Weinheimer; Jason C. Schroder; Pedro Campuzano-Jost; Douglas A. Day; Jose L. Jimenez; Jack E. Dibb; Teresa Campos; Viral Shah; Lyatt Jaeglé; Ronald C. Cohen

doi:10.1029/2018JD028736

NO_x Lifetime and NO_y Partitioning During WINTER

Hannah S. Kenagy, Tamara L. Sparks, Carlena J. Ebben, Paul J. Wooldrige, Felipe D. Lopez-Hilfiker, Ben H. Lee, Joel A. Thornton, Erin E. McDuffie, Dorothy L. Fibiger, Steven S. Brown, Denise D. Montzka, Andrew J. Weinheimer, Jason C. Schroder, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Jack E. Dibb, Teresa Campos, Viral Shah, Lyatt JaegléRonald C. Cohen

Research output: Contribution to journal › Article › peer-review

56 Scopus citations

Abstract

Although urban NO_x lifetimes have been examined extensively during summertime conditions, wintertime NO_x chemistry has been comparatively less studied. We use measurements of NO_x and its oxidation products from the aircraft-based WINTER (Wintertime INvestigation of Transport, Emissions, and Reactivity) experiment over the northeastern United States during February–March 2015 to describe the NO_x lifetime during conditions when days are shorter, actinic flux is reduced, and temperatures are colder. By analyzing regional outflow from the East Coast, we show that NO_x is long lived during the winter, with a longer daytime lifetime (29 hr) than nighttime lifetime (6.3 hr). We demonstrate that wintertime NO_x emissions have an overall lifetime controlled by the nighttime conversion of NO_x to nitric acid (HNO₃) via N₂O₅ heterogeneous chemistry, and we discuss constraints on the rates of NO_x conversion to HNO₃. Additionally, analysis of the nighttime O_x budget suggests that approximately 15% of O₃ is lost overnight through N₂O₅ production and subsequent reaction with aerosol to form HNO₃.

Original language	English (US)
Pages (from-to)	9813-9827
Number of pages	15
Journal	Journal of Geophysical Research: Atmospheres
Volume	123
Issue number	17
DOIs	https://doi.org/10.1029/2018JD028736
State	Published - Sep 16 2018
Externally published	Yes

Bibliographical note

Publisher Copyright:
©2018. American Geophysical Union. All Rights Reserved.

Keywords

NO
NO lifetime
WINTER
heterogeneous hydrolysis
nitric acid
winter

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10.1029/2018JD028736

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Kenagy, H. S., Sparks, T. L., Ebben, C. J., Wooldrige, P. J., Lopez-Hilfiker, F. D., Lee, B. H., Thornton, J. A., McDuffie, E. E., Fibiger, D. L., Brown, S. S., Montzka, D. D., Weinheimer, A. J., Schroder, J. C., Campuzano-Jost, P., Day, D. A., Jimenez, J. L., Dibb, J. E., Campos, T., Shah, V., ... Cohen, R. C. (2018). NO_x Lifetime and NO_y Partitioning During WINTER. Journal of Geophysical Research: Atmospheres, 123(17), 9813-9827. https://doi.org/10.1029/2018JD028736

Kenagy, HS, Sparks, TL, Ebben, CJ, Wooldrige, PJ, Lopez-Hilfiker, FD, Lee, BH, Thornton, JA, McDuffie, EE, Fibiger, DL, Brown, SS, Montzka, DD, Weinheimer, AJ, Schroder, JC, Campuzano-Jost, P, Day, DA, Jimenez, JL, Dibb, JE, Campos, T, Shah, V, Jaeglé, L & Cohen, RC 2018, 'NO_x Lifetime and NO_y Partitioning During WINTER', Journal of Geophysical Research: Atmospheres, vol. 123, no. 17, pp. 9813-9827. https://doi.org/10.1029/2018JD028736

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abstract = "Although urban NOx lifetimes have been examined extensively during summertime conditions, wintertime NOx chemistry has been comparatively less studied. We use measurements of NOx and its oxidation products from the aircraft-based WINTER (Wintertime INvestigation of Transport, Emissions, and Reactivity) experiment over the northeastern United States during February–March 2015 to describe the NOx lifetime during conditions when days are shorter, actinic flux is reduced, and temperatures are colder. By analyzing regional outflow from the East Coast, we show that NOx is long lived during the winter, with a longer daytime lifetime (29 hr) than nighttime lifetime (6.3 hr). We demonstrate that wintertime NOx emissions have an overall lifetime controlled by the nighttime conversion of NOx to nitric acid (HNO3) via N2O5 heterogeneous chemistry, and we discuss constraints on the rates of NOx conversion to HNO3. Additionally, analysis of the nighttime Ox budget suggests that approximately 15% of O3 is lost overnight through N2O5 production and subsequent reaction with aerosol to form HNO3.",

keywords = "NO, NO lifetime, WINTER, heterogeneous hydrolysis, nitric acid, winter",

author = "Kenagy, {Hannah S.} and Sparks, {Tamara L.} and Ebben, {Carlena J.} and Wooldrige, {Paul J.} and Lopez-Hilfiker, {Felipe D.} and Lee, {Ben H.} and Thornton, {Joel A.} and McDuffie, {Erin E.} and Fibiger, {Dorothy L.} and Brown, {Steven S.} and Montzka, {Denise D.} and Weinheimer, {Andrew J.} and Schroder, {Jason C.} and Pedro Campuzano-Jost and Day, {Douglas A.} and Jimenez, {Jose L.} and Dibb, {Jack E.} and Teresa Campos and Viral Shah and Lyatt Jaegl{\'e} and Cohen, {Ronald C.}",

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AU - Kenagy, Hannah S.

AU - Sparks, Tamara L.

AU - Ebben, Carlena J.

AU - Wooldrige, Paul J.

AU - Lopez-Hilfiker, Felipe D.

AU - Lee, Ben H.

AU - Thornton, Joel A.

AU - McDuffie, Erin E.

AU - Fibiger, Dorothy L.

AU - Brown, Steven S.

AU - Montzka, Denise D.

AU - Weinheimer, Andrew J.

AU - Schroder, Jason C.

AU - Campuzano-Jost, Pedro

AU - Day, Douglas A.

AU - Jimenez, Jose L.

AU - Dibb, Jack E.

AU - Campos, Teresa

AU - Shah, Viral

AU - Jaeglé, Lyatt

AU - Cohen, Ronald C.

PY - 2018/9/16

Y1 - 2018/9/16

N2 - Although urban NOx lifetimes have been examined extensively during summertime conditions, wintertime NOx chemistry has been comparatively less studied. We use measurements of NOx and its oxidation products from the aircraft-based WINTER (Wintertime INvestigation of Transport, Emissions, and Reactivity) experiment over the northeastern United States during February–March 2015 to describe the NOx lifetime during conditions when days are shorter, actinic flux is reduced, and temperatures are colder. By analyzing regional outflow from the East Coast, we show that NOx is long lived during the winter, with a longer daytime lifetime (29 hr) than nighttime lifetime (6.3 hr). We demonstrate that wintertime NOx emissions have an overall lifetime controlled by the nighttime conversion of NOx to nitric acid (HNO3) via N2O5 heterogeneous chemistry, and we discuss constraints on the rates of NOx conversion to HNO3. Additionally, analysis of the nighttime Ox budget suggests that approximately 15% of O3 is lost overnight through N2O5 production and subsequent reaction with aerosol to form HNO3.

AB - Although urban NOx lifetimes have been examined extensively during summertime conditions, wintertime NOx chemistry has been comparatively less studied. We use measurements of NOx and its oxidation products from the aircraft-based WINTER (Wintertime INvestigation of Transport, Emissions, and Reactivity) experiment over the northeastern United States during February–March 2015 to describe the NOx lifetime during conditions when days are shorter, actinic flux is reduced, and temperatures are colder. By analyzing regional outflow from the East Coast, we show that NOx is long lived during the winter, with a longer daytime lifetime (29 hr) than nighttime lifetime (6.3 hr). We demonstrate that wintertime NOx emissions have an overall lifetime controlled by the nighttime conversion of NOx to nitric acid (HNO3) via N2O5 heterogeneous chemistry, and we discuss constraints on the rates of NOx conversion to HNO3. Additionally, analysis of the nighttime Ox budget suggests that approximately 15% of O3 is lost overnight through N2O5 production and subsequent reaction with aerosol to form HNO3.

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KW - WINTER

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