A new insight into the vertical differences in NO2 heterogeneous reaction to produce HONO over inland and marginal seas
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Published:2023-05-26
Issue:10
Volume:23
Page:5815-5834
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Xing ChengzhiORCID, Xu Shiqi, Song YuhangORCID, Liu ChengORCID, Liu Yuhan, Lu KedingORCID, Tan Wei, Zhang ChengxinORCID, Hu Qihou, Wang Shanshan, Wu Hongyu, Lin Hua
Abstract
Abstract. Ship-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were conducted along the marginal seas of China from 19 April to 16 May 2018 to measure the vertical profiles of aerosol, nitrogen dioxide (NO2), and nitrous acid (HONO). Along the cruise route, we found five hot spots with enhanced tropospheric NO2 vertical column densities (VCDs) in the Yangtze River Delta, Taiwan Strait, Guangzhou–Hong Kong–Macau Greater Bay Area, port of Zhanjiang, and port of Qingdao. Enhanced HONO concentrations could
usually be observed under high-level aerosol and NO2 conditions,
whereas the reverse was not always the case. To understand the impacts of
relative humidity (RH), temperature, and aerosol on the heterogeneous
reaction of NO2 to form HONO in different scenarios, the Chinese Academy
of Meteorological Sciences (CAMS) and Southern University of Science and
Technology (SUST) MAX-DOAS stations were selected as the inland and coastal
cases, respectively. The RH turning points in CAMS and SUST cases were both
∼ 65 % (60 %–70 %), whereas two turning peaks
(∼ 60 % and ∼ 85 %) of RH were found in the
sea cases. As temperature increased, the HONO / NO2 ratio decreased with peak values appearing at ∼ 12.5∘C in CAMS, whereas the HONO / NO2 gradually increased and reached peak values at ∼ 31.5∘C in SUST. In the sea cases, when the temperature exceeded 18.0∘C, the HONO / NO2 ratio rose with increasing temperature and
achieved its peak at ∼ 25.0∘C. This indicated that
high temperature can contribute to the secondary formation of HONO in the
sea atmosphere. In the inland cases, the correlation analysis between HONO
and aerosol in the near-surface layer showed that the ground surface is more crucial to the formation of HONO via the heterogeneous reaction of NO2; however, in the coastal and sea cases, the aerosol surface contributed more. Furthermore, we discovered that the conversion rate of NO2 to HONO through heterogeneous reactions in the sea cases is larger than that in the inland cases in higher atmospheric layers (> 600 m). Three typical events were selected to demonstrate three potential contributing factors of
HONO production under marine conditions (i.e., transport, NO2
heterogeneous reaction, and unknown HONO source). This study elucidates the
sea–land and vertical differences in the forming mechanism of HONO via the
NO2 heterogeneous reaction and provides deep insights into tropospheric HONO distribution, transforming process, and environmental effects.
Funder
National Natural Science Foundation of China Natural Science Foundation of Anhui Province Hefei Institutes of Physical Science, Chinese Academy of Sciences Chinese Academy of Sciences
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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