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Discussion papers | Copyright
https://doi.org/10.5194/acp-2018-334
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 14 May 2018

Research article | 14 May 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Atmospheric Δ17O(NO3) reveals nocturnal chemistry dominates nitrate production in Beijing haze

Pengzhen He1, Zhouqing Xie1,2,3, Xiyuan Chi1, Xiawei Yu1, Shidong Fan1, Hui Kang1, Cheng Liu1,2,3, and Haicong Zhan1 Pengzhen He et al.
  • 1Anhui Province Key Laboratory of Polar Environment and Global Change, School of Earth and Space Sciences, University of Science and Technology of China, Hefei, Anhui 230026, China
  • 2Key Lab of Environmental Optics and Technology, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei, Anhui 230031, China
  • 3Center for Excellence in Urban Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, Fujian 361021, China

Abstract. The rapid mass increase of atmospheric nitrate is a critical driving force for the occurrence of fine-particle pollution (referred to as haze hereafter) in Beijing. However, the exact mechanisms for this rapid increase of nitrate mass has been not well constrained from field observations. Here we present the first observations of the oxygen-17 excess of atmospheric nitrate (Δ17O(NO3)) collected in Beijing haze to reveal the relative importance of different nitrate formation pathways, and we also present the simultaneously observed δ15N(NO3). During our sampling period, 12h-averaged mass concentrations of PM2.5 varied from 16 to 323μgm−3 with a mean of (141±88 (1σ))μgm−3, with nitrate ranging from 0.3 to 106.7μgm−3. The observed Δ17O(NO3) ranged from 27.5‰ to 33.9‰ with a mean of (30.6±1.8)‰ while δ15N(NO3) ranged from −2.5‰ to 19.2‰ with a mean of (7.4±6.8)‰. Δ17O(NO3)-constrained calculations suggest nocturnal pathways (N2O5 + H2O/Cl and NO3 + HC) dominated nitrate production during polluted days (PM2.5 ≥ 75μgm−3) with the mean possible fraction of 56 − 97%. For δ15N(NO3), we found that a combined effect of variability in NOX sources and isotopic exchange between NO and NO2 is likely to be most responsible for its variations. Our results illustrate the potentiality of isotope in tracing NOX sources and nitrate formation pathways, future modelling work with the constraint of isotope data reported here may further improve our understanding of nitrogen cycle during haze.

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The rapid mass increase of atmospheric nitrate is a critical driving force for the occurrence of fine-particle pollution (referred to as haze hereafter) in Beijing. However, the exact mechanisms for this rapid increase of nitrate mass has been not well constrained from field observations. Here we present the first observations of the oxygen-17 excess of atmospheric nitrate (Δ17O(NO3)) collected in Beijing haze to reveal the relative importance of different nitrate formation pathways.
The rapid mass increase of atmospheric nitrate is a critical driving force for the occurrence of...
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