Romer, Paul S. and Wooldridge, Paul J. and Crounse, John D. and Kim, Michelle J. and Wennberg, Paul O. and Dibb, Jack E. and Scheuer, Eric and Blake, Donald R. and Meinardi, Simone and Brosius, Alexandra L. and Thames, Alexander B. and Miller, David O. and Brune, William H. and Hall, Samuel R. and Ryerson, Thomas B. and Cohen, Ronald C. (2018) Constraints on aerosol nitrate photolysis as a potential source of HONO and NO_x. Environmental Science and Technology, 52 (23). pp. 13738-13746. ISSN 0013-936X. doi:10.1021/acs.est.8b03861. https://resolver.caltech.edu/CaltechAUTHORS:20181113-112610113
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Abstract
The concentration of nitrogen oxides (NO_x) plays a central role in controlling air quality. On a global scale, the primary sink of NO_x is oxidation to form HNO_3. Gas-phase HNO_3 photolyses slowly with a lifetime in the troposphere of 10 days or more. However, several recent studies examining HONO chemistry have proposed that particle-phase HNO_3 undergoes photolysis 10–300 times more rapidly than gas-phase HNO_3. We present here constraints on the rate of particle-phase HNO_3 photolysis based on observations of NO_x and HNO_3 collected over the Yellow Sea during the KORUS-AQ study in summer 2016. The fastest proposed photolysis rates are inconsistent with the observed NO_x to HNO_3 ratios. Negligible to moderate enhancements of the HNO_3 photolysis rate in particles, 1–30 times faster than in the gas phase, are most consistent with the observations. Small or moderate enhancement of particle-phase HNO_3 photolysis would not significantly affect the HNO_3 budget but could help explain observations of HONO and NO_x in highly aged air.
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| Alternate Title: | Constraints on aerosol nitrate photolysis as a potential source of HONO and NOx | ||||||||||||||||||||||||||||||
| Additional Information: | © 2018 American Chemical Society. Received: July 13, 2018; Revised: October 22, 2018; Accepted: November 8, 2018; Published: November 8, 2018. We thank NASA for support via NNX15AT85G (Berkeley), NNX15AT97G and NNX14AP46G (Caltech), NNX14AP46G (UNH), and NNX16AD96G (to C.K.). M.J.K. was supported by NSF AGS Award No. 1524860. Methanol and acetaldehyde measurements were supported by the Austrian Federal Ministry for Transport, Innovation and Technology (bmvit) through the Austrian Research Promotion Agency (FFG). The authors thank Alan Fried for the formaldehyde measurements, Armin Wisthaler for the methanol and acetaldehyde measurements, Christoph Knote for the FLEXPART model results, Glenn Diskin for the CH4 and CO measurements, and Andrew Weinheimer and Denise Montzka for NO measurements. We thank Tamara Sparks and Alex Teng for assistance in the field, the ground and flight crew of the DC-8, and the KORUS-AQ science team. The authors declare no competing financial interest. | ||||||||||||||||||||||||||||||
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| Issue or Number: | 23 | ||||||||||||||||||||||||||||||
| DOI: | 10.1021/acs.est.8b03861 | ||||||||||||||||||||||||||||||
| Record Number: | CaltechAUTHORS:20181113-112610113 | ||||||||||||||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20181113-112610113 | ||||||||||||||||||||||||||||||
| Official Citation: | Constraints on Aerosol Nitrate Photolysis as a Potential Source of HONO and NOx. Paul S. Romer, Paul J. Wooldridge, John D. Crounse, Michelle J. Kim, Paul O. Wennberg, Jack E. Dibb, Eric Scheuer, Donald R. Blake, Simone Meinardi, Alexandra L. Brosius, Alexander B. Thames, David O. Miller, William H. Brune, Samuel R. Hall, Thomas B. Ryerson, and Ronald C. Cohen. Environmental Science & Technology 2018 52 (23), 13738-13746 DOI: 10.1021/acs.est.8b03861 | ||||||||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||||||||
| ID Code: | 90872 | ||||||||||||||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||||||||||||||
| Deposited By: | George Porter | ||||||||||||||||||||||||||||||
| Deposited On: | 13 Nov 2018 21:12 | ||||||||||||||||||||||||||||||
| Last Modified: | 16 Nov 2021 03:36 |
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