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Combined Impacts of Nitrous Acid and Nitryl Chloride On Lower-tropospheric Ozone: New Module Development In WRF-CHEM and Application To China

Abstract

Nitrous acid (HONO) and nitryl chloride (ClNO2) – through their photolysis – can have profound effects on the nitrogen cycle and oxidation capacity of the lower troposphere. Previous numerical studies have separately considered and investigated the sources/processes of these compounds and their roles in the fate of reactive nitrogen and the production of ozone (O3), but their combined impact on the chemistry of the lower part of the troposphere has not been addressed yet. In this study, we updated the WRF-Chem model with the currently known sources and chemistry of HONO and chlorine in a new chemical mechanism (CBMZ_ReNOM), and applied it to a study of the combined effects of HONO and ClNO2 on summertime O3 in the boundary layer over China. We simulated the spatial distributions of HONO, ClNO2, and related compounds at the surface and within the lower troposphere. The results showed that the modeled HONO levels reached up to 800–1800 ppt at the surface (0–30 m) over the North China Plain (NCP), the Yangtze River Delta (YRD), and the Pearl River Delta (PRD) regions and that HONO was concentrated within a 0–200 m layer. In comparison, the simulated surface ClNO2 mixing ratio was around 800–1500 ppt over the NCP, YRD, and central China regions and was predominantly present in a 0–600 m layer. HONO enhanced daytime ROx (OH + HO2 + RO2) and O3 at the surface (0–30 m) by 2.8–4.6 ppt (28–37 %) and 2.9–6.2 ppb (6–13 %), respectively, over the three most developed regions, whereas ClNO2 increased surface O3 in the NCP and YRD regions by 2.4–3.3 ppb (or 5–6 %) and it also had a significant impact (3–6 %) on above-surface O3 within 200–500 m. The combined effects increased surface O3 by 11.5, 13.5, and 13.3 % in the NCP, YRD, and PRD regions, respectively. Over the boundary layer (0–1000 m), the HONO and ClNO2 enhanced O3 by up to 5.1 and 3.2 %, respectively, and their combined effect increased O3 by 7.1–8.9 % in the three regions. The new module noticeably improved O3 predictions at ∼ 900 monitoring stations throughout China by reducing the mean bias from −4.3 to 0.1 ppb. Our study suggests the importance of considering these reactive nitrogen species simultaneously into chemical transport models to better simulate the formation of summertime O3 in polluted regions.

Article / Publication Data
Active/Online
YES
Volume
17
Available Metadata
Accepted On
July 16, 2017
DOI ↗
Fiscal Year
NOAA IR URL ↗
Peer Reviewed
YES
Publication Name
Atmospheric Chemistry and Physics
Published On
August 17, 2017
Publisher Name
European Geophysical Union
Print Volume
17
Print Number
16
Page Range
9733-9750
Issue
16
Submitted On
April 27, 2017
URL ↗

Authors

Authors who have authored or contributed to this publication.

  • Li (Kate) Zhang - lead Gsl
    Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder
    NOAA/Global Systems Laboratory
  • Ravan Ahmadov - fourth Gsl
    Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder
    NOAA/Global Systems Laboratory