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Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain

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Author(s)

  • Yuk-Chun Chan
  • Mathew J. Evans
  • Pengzhen He
  • Christopher D. Holmes
  • Lyatt Jaeglé
  • Prasad Kasibhatla
  • Xue-Yan Liu
  • Tomás Sherwen
  • Joel A. Thornton
  • Xuan Wang
  • Zhouqing Xie
  • Shuting Zhai
  • Becky Alexander

Department/unit(s)

Publication details

JournalJournal of Geophysical Research: Atmospheres
DateAccepted/In press - 21 Apr 2021
DatePublished (current) - 5 May 2021
Issue number9
Volume126
Original languageEnglish

Abstract

Abstract Studies of wintertime air quality in the North China Plain (NCP) show that particulate-nitrate pollution persists despite rapid reduction in NOx emissions. This intriguing NOx-nitrate relationship may originate from non-linear nitrate-formation chemistry, but it is unclear which feedback mechanisms dominate in NCP. In this study, we re-interpret the wintertime observations of 17O excess of nitrate (∆17O(NO3−)) in Beijing using the GEOS-Chem (GC) chemical transport model to estimate the importance of various nitrate-production pathways and how their contributions change with the intensity of haze events. We also analyze the relationships between other metrics of NOy chemistry and [PM2.5] in observations and model simulations. We find that the model on average has a negative bias of −0.9‰ and −3617O(NO3−) and [Ox,major] (≡ [O3] + [NO2] + [p-NO3−]), respectively, while overestimating the nitrogen oxidation ratio ([NO3−]/([NO3−] + [NO2])) by +0.12 in intense haze. The discrepancies become larger in more intense haze. We attribute the model biases to an overestimate of NO2-uptake on aerosols and an underestimate in wintertime O3 concentrations. Our findings highlight a need to address uncertainties related to heterogeneous chemistry of NO2 in air-quality models. The combined assessment of observations and model results suggest that N2O5 uptake in aerosols and clouds is the dominant nitrate-production pathway in wintertime Beijing, but its rate is limited by ozone under high-NOx-high-PM2.5 conditions. Nitrate production rates may continue to increase as long as [O3] increases despite reduction in [NOx], creating a negative feedback that reduces the effectiveness of air pollution mitigation.

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    Research areas

  • Δ17O(NO3−), GEOS-Chem, heterogeneous chemistry, nitrate, NO2 uptake, winter air quality

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