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https://doi.org/10.5194/acp-2020-377
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-377
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 25 May 2020

Submitted as: research article | 25 May 2020

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This preprint is currently under review for the journal ACP.

Sources of nitrous acid (HONO) in the upper boundary layer and lower free troposphere of North China Plain: insights from the Mount Tai Observatory

Ying Jiang1, Likun Xue1,4, Rongrong Gu1, Mengwei Jia2, Yingnan Zhang1, Liang Wen1, Penggang Zheng1, Tianshu Chen1, Hongyong Li1, Ye Shan1, Yong Zhao3, Zhaoxin Guo3, Yujian Bi3, Hengde Liu3, Aijun Ding2,4, Qingzhu Zhang1, and Wenxing Wang1 Ying Jiang et al.
  • 1Environment Research Institute, Shandong University, Qingdao, Shandong, 266237, China
  • 2School of Atmospheric Sciences, Nanjing University, Nanjing, 210023, China
  • 3Taishan National Reference Climatological Station, Tai'an, Shandong, 271000, China
  • 4Collaborative innovation Center for climate Change, Jiangsu Province, Nanjing, 210023, China

Abstract. Nitrous acid (HONO) is a significant precursor of atmospheric detergent OH radicals, and plays a vital role in tropospheric chemistry. The current knowledge about the daytime HONO sources is incomplete, and its impact on the tropospheric radical chemistry has not been fully quantified. Existing observational studies of HONO were mostly conducted at surface, with few efforts focusing on the high-elevation atmospheres. In order to better understand the characteristics and sources of HONO in the upper boundary layer and lower free troposphere, two intensive field observations were carried out at the summit of Mt. Tai (1534 m a.s.l.), the peak of the North China Plain, in winter 2017 and spring 2018. HONO showed moderate concentration levels (0.15 ± 0.15 and 0.13 ± 0.15 ppbv), with maximum values of 1.14 and 3.23 ppbv in winter and spring, respectively. Diurnal variation patterns with a broad noontime maximum and lower nighttime concentrations were observed during both campaigns, which is distinct from most of the previous studies at the ground level. The WRF-FLEXPART simulations indicated the combined effects of the planetary boundary layer evolution and valley breeze on the daytime HONO peak. A photostationary state (PSS) analysis suggested the strong unknown daytime HONO source with production rates of 0.45 ± 0.25 ppb/h in winter and 0.64 ± 0.49 ppb/h in spring. Correlation analysis supported the important role of photo-enhanced heterogeneous conversion of NO2 to HONO on the aerosol surface at this high-elevation site. HONO photolysis is the predominant primary source of OH radical and plays a major role in the radical chemistry at Mt. Tai. The model only considering homogenous HONO source would largely underestimate the HOx radical levels and atmospheric oxidation capacity in the high-altitude atmosphere. This study shed light on the characteristics, sources, chemistry, and impacts of HONO in the upper boundary layer and lower free troposphere in the NCP region.

Ying Jiang et al.

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Short summary
We analyzed the characteristics and sources of HONO in the upper boundary layer and lower free troposphere in the North China Plain, based on the field measurements at Mt. Tai. Higher than expected levels and broad daytime peaks of HONO were observed. Without presence of ground surfaces, aerosol surface plays a key role in the heterogeneous HONO formation at high altitudes. Models without additional HONO sources largely underestimated the oxidation processes in the elevation atmospheres.
We analyzed the characteristics and sources of HONO in the upper boundary layer and lower free...
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