Preprints
https://doi.org/10.5194/acp-2022-638
https://doi.org/10.5194/acp-2022-638
 
01 Nov 2022
01 Nov 2022
Status: this preprint is currently under review for the journal ACP.

A new insight of the vertical differences of NO2 heterogeneous reaction to produce HONO over inland and marginal seas

Chengzhi Xing1, Shiqi Xu7, Cheng Liu2,1,3,4, Yuhan Liu6, Keding Lu5, Wei Tan1, Qihou Hu1, Shanshan Wang9, Hongyu Wu8, and Hua Lin8 Chengzhi Xing et al.
  • 1Key Lab of Environmental Optics & Technology, Anhui Institute of Optics and Fine Mechanics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
  • 2Department of Precision Machinery and Precision Instrumentation, University of Science and Technology of China, Hefei, 230026, China
  • 3Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China
  • 4Key Laboratory of Precision Scientific Instrumentation of Anhui Higher Education Institutes, University of Science and Technology of China, Hefei, 230026, China
  • 5State Key Joint Laboratory of Environment Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
  • 6Department of unclear safety, Chia Institute of Atomic Energy, Beijing, 102413, China
  • 7School of Earth and Space Sciences, University of Science and Technology of China, Hefei, 230026, China
  • 8School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei, 230026, China
  • 9Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai, 200433, China

Abstract. Ship based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were carried out along the marginal seas of China from 19 April to 16 May 2018, to measures the vertical profiles of aerosol, NO2 and HONO. Five hot spots of tropospheric NO2 VCDs were found in Yangtze River Delta, Taiwan straits, Guangzhou-Hong Kong-Macao Greater Bay areas, Zhanjiang Port, and Qingdao port with averaged NO2 VCDs of 1.07×1016, 1.30×1016, 7.27×1015, 5.34×1015, and 3.12×1015 molec. cm-2, respectively. HONO performs similar spatial distribution characteristics as NO2 with averaged HONO VCDs in above five hot-spot areas of 1.01×1015, 7.91×1014, 6.02×1014, 5.36×1014, and 5.17×1014 molec. cm-2, respectively. The averaged near-surface NO2 concentrations were 8.46 and 11.31 ppb, and the averaged near-surface HONO concentrations were 0.23 and 0.27 ppb under viewing sea and viewing land observation azimuths during the whole campaign, respectively. The Chinese Academy of Meteorological Sciences (CAMS) and Southern University of Science and Technology (SUST) MAX-DOAS stations were selected as inland and coastal cases to further understand the impacts of relative humidity (RH), temperature, and solar radiation intensity (SRI) on the heterogeneous reaction of NO2 to form HONO in different scenes. The emission ratios of ΔHONO / ΔNOx in sea, CAMS and SUST were 0.46±0.31 %, 0.82±0.34 %, and 0.79±0.31 %, respectively. The RH turning points in CAMS and SUST cases were all ~65 % (60–70 %), however, two turning peaks (~60 % and ~85 %) of RH were found in sea cases. The HONO/NO2 decrease along with the increase of temperature, and with peak values on ~12.5 °C in CAMS. The HONO/NO2 increase along with increasing temperature, and with peak values on ~31.5 °C in SUST. In sea case, the HONO/NO2 increase along with the increase of temperature with a peak value on ~25.0 °C under the temperature being larger than 18.0 °C. That means the high temperature could contribute to the secondary formation of HONO in sea atmosphere. The correlation analysis between HONO and aerosol in near-surface layer illustrated the ground surface plays a more important role than aerosol surface during the HONO formation process from the heterogeneous reaction of NO2 under inland case, however, aerosol surface plays a more important role during above process under coastal and sea cases. Moreover, we found the HONO generation rate from NO2 heterogeneous reaction in sea case is larger than that in inland case in higher atmospheric layers above 600 m.

Chengzhi Xing et al.

Status: open (until 13 Dec 2022)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • CC1: 'Comment on acp-2022-638', Jörg Kleffmann, 09 Nov 2022 reply
  • RC1: 'Comment on acp-2022-638', Anonymous Referee #1, 11 Nov 2022 reply

Chengzhi Xing et al.

Chengzhi Xing et al.

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Short summary
High RH could contribute to the secondary formation of HONO in sea atmosphere. High temperature could promote the formation of HONO from NO2 heterogeneous reaction in sea and coastal atmosphere. Aerosol surface plays a more important role during above process under coastal and sea cases. The generation rate of HONO from NO2 heterogeneous reaction in sea case is larger than that in inland cases in higher atmospheric layers above 600 m.
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