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<article xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:oasis="http://docs.oasis-open.org/ns/oasis-exchange/table" xml:lang="en" dtd-version="3.0" article-type="research-article"><?xmltex \hack{\hyphenation{indicating}}?><?xmltex \hack{\hyphenation{considerable}}?><?xmltex \hack{\hyphenation{platform}}?><?xmltex \bartext{Research article}?>
  <front>
    <journal-meta><journal-id journal-id-type="publisher">ACP</journal-id><journal-title-group>
    <journal-title>Atmospheric Chemistry and Physics</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1680-7324</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-22-14455-2022</article-id><title-group><article-title>What caused ozone pollution during the 2022 Shanghai lockdown? Insights from ground and satellite observations</article-title><alt-title>Ozone pollution during the 2022 Shanghai lockdown</alt-title>
      </title-group><?xmltex \runningtitle{Ozone pollution during the 2022 Shanghai lockdown}?><?xmltex \runningauthor{Y. Tan and T. Wang}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="no">
          <name><surname>Tan</surname><given-names>Yue</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="yes">
          <name><surname>Wang</surname><given-names>Tao</given-names></name>
          <email>tao.wang@polyu.edu.hk</email>
        <ext-link>https://orcid.org/0000-0002-4765-9377</ext-link></contrib>
        <aff id="aff1"><institution>Department of Civil and Environmental Engineering, The Hong Kong Polytechnic
University,<?xmltex \hack{\break}?> Hong Kong, 999077, China</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Tao Wang (tao.wang@polyu.edu.hk)</corresp></author-notes><pub-date><day>14</day><month>November</month><year>2022</year></pub-date>
      
      <volume>22</volume>
      <issue>22</issue>
      <fpage>14455</fpage><lpage>14466</lpage>
      <history>
        <date date-type="received"><day>2</day><month>August</month><year>2022</year></date>
           <date date-type="rev-request"><day>24</day><month>August</month><year>2022</year></date>
           <date date-type="rev-recd"><day>24</day><month>October</month><year>2022</year></date>
           <date date-type="accepted"><day>25</day><month>October</month><year>2022</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2022 </copyright-statement>
        <copyright-year>2022</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d1e93">Shanghai, one of China's most important economic centres, imposed a citywide lockdown in April and May 2022 to contain a resurgence in cases of the coronavirus disease in 2019. Compared with the 2020 lockdown, the 2022 lockdown occurred in a warm season and lasted much longer, thereby serving
as a relevant real-world test of the response of ambient ozone (O<inline-formula><mml:math id="M1" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>)
concentrations to emission reductions in a high-O<inline-formula><mml:math id="M2" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> season. In this
study, we analysed surface observations of O<inline-formula><mml:math id="M3" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and nitrogen dioxide
(NO<inline-formula><mml:math id="M4" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>) concentrations and satellite-retrieved tropospheric NO<inline-formula><mml:math id="M5" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and
formaldehyde (HCHO) column concentrations in the first 5 months of 2022 with comparisons to the year 2021. During the 2-month 2022 lockdown, the maximum daily 8 h average (MDA8) O<inline-formula><mml:math id="M6" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations at 1 or more of the city's 19 sites exceeded China's air quality standard of 160 <inline-formula><mml:math id="M7" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> 21 times, with the highest value being 200 <inline-formula><mml:math id="M8" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. The city-average MDA8 O<inline-formula><mml:math id="M9" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration increased by 13 % in April–May 2022 year-on-year, despite sharp declines in NO<inline-formula><mml:math id="M10" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> surface and column concentrations (both by 49 %) and a 19 % decrease in the HCHO column concentration. These results show that the reductions in O<inline-formula><mml:math id="M11" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> precursors and other pollutants during the 2022 lockdown did not prevent ground-level O<inline-formula><mml:math id="M12" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution. An analysis of meteorological data indicates that there were only small changes in the meteorological conditions, and there was little transport of O<inline-formula><mml:math id="M13" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> from the high-O<inline-formula><mml:math id="M14" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> inland regions during the 2022 lockdown, neither of which can account for the increased and high concentrations of O<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> that were observed during this period. The mean <inline-formula><mml:math id="M16" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio in April–May increased from 1.11 in 2021 to 1.68 in 2022, and the correlation between surface O<inline-formula><mml:math id="M17" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M18" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations changed from negative in 2021 to positive in 2022. These results indicate that the high O<inline-formula><mml:math id="M19" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations in 2022 were mainly due to large reductions in the emissions of <inline-formula><mml:math id="M20" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and that the decrease in the concentrations of volatile organic compounds (VOCs) could not overcome the NO titration effect. During the 2022 lockdown, Shanghai's urban centre remained VOC-sensitive despite drastic reductions in road transportation (73 %–85 %) and industrial activities (<inline-formula><mml:math id="M21" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">60</mml:mn></mml:mrow></mml:math></inline-formula> %), whereas its semi-rural areas transitioned from VOC-limited to
VOC–<inline-formula><mml:math id="M22" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-co-limited regimes. Our findings suggest that future emission
reductions similar to those that occurred during the lockdown, such as those
that will result from electrifying transportation, will not be sufficient to
eliminate O<inline-formula><mml:math id="M23" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution in urban areas of Shanghai and possibly other
VOC-limited metropoles without the imposition of additional VOC controls or
more substantial decreases in <inline-formula><mml:math id="M24" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emissions.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e358">Shanghai is a megacity with over 25 million residents and a land area of
6341 km<inline-formula><mml:math id="M25" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>. It serves as a financial, transport and logistics centre of
mainland China. From 27 March to 1 June 2022, the city imposed a strict
2-month lockdown (LCD) to curb increases in the number of cases of
the coronavirus disease in 2019 (COVID-19). Official statistics indicate that both
economic activities and human livelihood were severely disrupted by the 2022
Shanghai LCD (hereinafter “2022 LCD”). For example, in April, year-on-year
road passenger traffic turnover decreased by 85.5 %, and road cargo
turnover decreased by 73.1 % (Shanghai Bureau of Statistics, 2022); total industrial output decreased by 61.6 %, and power generation
decreased by 41.7 % (National Bureau of Statistics, 2022); and
port cargo throughput at the Port of Shanghai, the world's largest seaport,
decreased by 36.5 % (Ministry of Transport of the People's
Republic of China, 2022). As Shanghai is the most important transportation
and logistics hub of the manufacturing-intensive Yangtze River Delta (YRD)
region, the ripple effects of the LCD in Shanghai have disrupted supply
chains of its surrounding provinces, other regions of China and the world
(Cao et al., 2022; Hale et al., 2022; He, 2022).</p>
      <p id="d1e370">Such a reduction in human activity can be expected to drastically decrease
emissions of air pollutants, as has been borne out by numerous studies of
the 2020 LCD (Wang et al., 2022; Huang et al., 2021; Doumbia et al., 2021). Compared with the
2020 LCD in China, which was imposed in late January–early February, the
2022 LCD in Shanghai was imposed in the high-O<inline-formula><mml:math id="M26" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> season and lasted for
longer, during which time the O<inline-formula><mml:math id="M27" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations exceeding the air
quality standard were frequently observed. In the present study, we aimed to
understand how meteorology and non-linear chemistry influenced ground-level
O<inline-formula><mml:math id="M28" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations during the 2022 LCD and whether the huge decrease in
<inline-formula><mml:math id="M29" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emission could push a typical volatile organic compound (VOC)-limited megacity to a
<inline-formula><mml:math id="M30" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-limited regime. We first analysed surface observations of O<inline-formula><mml:math id="M31" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M32" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations and satellite-measured NO<inline-formula><mml:math id="M33" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and HCHO column concentrations to assess changes in the concentrations of these species in Shanghai and its surrounding areas during the 2022 LCD. We then examined the roles of meteorological and chemical conditions in determining O<inline-formula><mml:math id="M34" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations during the 2022 LCD by analysing small- and large-scale
meteorological data and chemical indicators of O<inline-formula><mml:math id="M35" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> formation regimes. We
discuss the implications of our findings for future strategies aimed at
reducing O<inline-formula><mml:math id="M36" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations, which is currently the dominant air
pollutant in China in warm seasons.</p><?xmltex \hack{\newpage}?>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Data and methodology</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Surface measurement data</title>
      <p id="d1e493">We obtained hourly concentrations of ground-level O<inline-formula><mml:math id="M37" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>, NO<inline-formula><mml:math id="M38" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, and
particulate matter of 2.5 <inline-formula><mml:math id="M39" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and smaller (PM<inline-formula><mml:math id="M40" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>) recorded at
<inline-formula><mml:math id="M41" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1700</mml:mn></mml:mrow></mml:math></inline-formula> stations in China during 2019–2022 from the China
National Environmental Monitoring Centre (<uri>https://quotsoft.net/air/</uri>, last access: 5 July 2022). The ambient concentrations of O<inline-formula><mml:math id="M42" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>,
NO<inline-formula><mml:math id="M43" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M44" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> are measured by an automated monitoring system at
each site and reported to the China National Environmental Monitoring Centre
and published online after validation (Wang et al., 2014). O<inline-formula><mml:math id="M45" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>,
NO<inline-formula><mml:math id="M46" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M47" display="inline"><mml:msub><mml:mi/><mml:mrow><mml:mn mathvariant="normal">2.5</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/></mml:mrow></mml:msub></mml:math></inline-formula>are measured with UV photometry,
chemiluminescence, and micro-oscillating balance or <inline-formula><mml:math id="M48" display="inline"><mml:mi mathvariant="italic">β</mml:mi></mml:math></inline-formula> absorption,
respectively, with a detection limit of 2 ppb, 2 ppb and 2 <inline-formula><mml:math id="M49" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, respectively (<uri>https://www.mee.gov.cn/</uri>, last access: 15 September 2022). The national network has 10 stations in Shanghai in 2019–2020, most of which are situated within the city centre. Since 2021, the number of stations has increased to 20, with most newly added sites located outside the city centre (refer to Figs. 1 and S1 in the Supplement for their locations). (Note there were no data from one site (Dianshanhu) in 2021–2022; thus the data from 19 stations are available for the years 2021 and 2022). The maximum daily 8 h average (MDA8) O<inline-formula><mml:math id="M50" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration was calculated for each site as the highest value of the 24 8 h moving average O<inline-formula><mml:math id="M51" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations for a given day. The daily average concentrations of the other pollutants (NO<inline-formula><mml:math id="M52" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and PM<inline-formula><mml:math id="M53" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula>) were also calculated from the hourly data. The 14 d moving averages of the surface
pollutant concentrations were calculated, as these had fewer fluctuations
than daily concentrations and thus better revealed trends. Finally, the
daily average mixing ratios of <inline-formula><mml:math id="M54" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:mo>=</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula>) were calculated to account for the titration effect of nitric oxide (NO) on
changes in O<inline-formula><mml:math id="M56" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e714">Spatial distribution and classification of the 20 environmental
monitoring sites in Shanghai. Types A, B, C and D represent sites in the
city centre (12 sites, circles), city perimeter (5 sites, squares),
semi-rural area (2 sites, diamonds) and the Yangtze River Estuary (1
site, cross), respectively.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f01.png"/>

        </fig>

</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Satellite and meteorological data</title>
      <p id="d1e731">Satellite data were used to investigate the spatiotemporal variations in
tropospheric formaldehyde (HCHO) and NO<inline-formula><mml:math id="M57" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> column concentrations during
the 2022 LCD period and the same period in 2021. We obtained Sentinel-5P
Level 3 offline products (HCHO and NO<inline-formula><mml:math id="M58" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>) using the TROPOspheric
Monitoring Instrument (TROPOMI) from the Google Earth Engine (GEE;
<uri>https://earthengine.google.com/</uri>, last access: 19 July 2022) cloud-based platform, which is
an open-source processing system based on JavaScript (Ghasempour et al., 2021). The Sentinel-5P Level 3 offline products were converted from the original Sentinel-5P Level 2 offline data (at a resolution of <inline-formula><mml:math id="M59" display="inline"><mml:mrow><mml:mn mathvariant="normal">5.5</mml:mn><mml:mo>×</mml:mo><mml:mn mathvariant="normal">3.5</mml:mn></mml:mrow></mml:math></inline-formula> km) by GEE using the harpconvert tool
(<uri>https://cdn.rawgit.com/stcorp/harp/master/doc/html/harpconvert.html</uri>, last access: 19 July 2022) and
subjected to a data quality control process, in which pixels with data
quality values less than 75 % for NO<inline-formula><mml:math id="M60" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and less than 50 % for HCHO
were removed. Based on the GEE platform, we imported the daily image
collections of HCHO and NO<inline-formula><mml:math id="M61" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, cut them in accordance with the
administrative boundary shapefiles of Shanghai (generated from publicly
available geoscience data on the DataV.GeoAtlas platform; <uri>http://datav.aliyun.com/portal/school/atlas/area_generator</uri>, last access: 19 July 2022)
using a <italic>.clip()</italic> script (Gorelick et al., 2017), and then averaged
the values of all the remaining pixels within the city border to obtain the
daily mean concentrations of HCHO and NO<inline-formula><mml:math id="M62" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>. A similar satellite data
processing method was used for the YRD region.</p>
      <p id="d1e804">We acquired surface site meteorological data (2 m temperature, 2 m relative
humidity (RH), 10 m wind direction and 10 m wind speed) from 78 weather
stations in Shanghai during April–May in 2021 and 2022, together with
gridded meteorological data (2 m temperature, 1000 hPa RH, downward
ultraviolet (UV) radiation at the surface, total cloud cover, total
precipitation and boundary layer height) from European Centre for
Medium-Range Weather Forecast reanalysis v5 (ERA5) (<uri>https://cds.climate.copernicus.eu/cdsapp#!/dataset/reanalysis-era5-single-levels</uri>, last access: 12 July 2022;
<uri>https://cds.climate.copernicus.eu/cdsapp#!/dataset/reanalysis-era5-pressure-levels</uri>, last access: 12 July 2022).
We calculated monthly averages of the surface-observed meteorological data
in 2021 and 2022 and the changes in gridded meteorological data between 2022
and 2021 to determine the spatiotemporal variations in meteorological
conditions in Shanghai and its surrounding regions.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Backward trajectory analysis</title>
      <p id="d1e821">The 24 h backward trajectories for Shanghai were calculated at 1 h intervals during April–May 2022 using MeteoInfoMap software (Wang, 2014, 2019) and meteorological data from the Global Data Assimilation System (<uri>ftp://arlftp.arlhq.noaa.gov/pub/archives/gdas1/</uri>, last access: 18 July 2022). The endpoints of the trajectories were 500 m above ground level of Shanghai (31.23<inline-formula><mml:math id="M63" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 121.47<inline-formula><mml:math id="M64" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E). Cluster classification was then conducted to divide the trajectories of O<inline-formula><mml:math id="M65" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> exceedance days into five groups based on the origins of air mass.</p><?xmltex \hack{\newpage}?>
</sec>
<sec id="Ch1.S2.SS4">
  <label>2.4</label><title>Site classification and regression analysis</title>
      <p id="d1e863">We classified the aforementioned 19 environmental monitoring sites in
Shanghai into 4 types based on land use and mean <inline-formula><mml:math id="M66" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios
(Figs. 1 and 8b). The type A sites (12 sites) are in the city centre
(and almost all are within the Shanghai Outer Ring Expressway) and had the
lowest <inline-formula><mml:math id="M67" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios; type B sites are sites in the city perimeter (4 sites) that had moderate <inline-formula><mml:math id="M68" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios; type C sites are semi-rural sites (2 sites) that had the largest <inline-formula><mml:math id="M69" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios; and the type D site (1 site) is located near the wetland park in the East Chongming Tidal Flat and is least affected by urban emissions but may be influenced by ship
emissions. Based on the above classification, we conducted regression
analyses between the surface MDA8 O<inline-formula><mml:math id="M70" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations and daily mean
NO<inline-formula><mml:math id="M71" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations for three types of sites (A, B and C) to examine the
O<inline-formula><mml:math id="M72" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> formation regime during the 2022 LCD in Shanghai's city centre and city
perimeter and at semi-rural sites.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results and discussion</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><?xmltex \opttitle{Spatiotemporal variations in surface MDA8 O${}_{{3}}$ and NO${}_{{2}}$
concentrations}?><title>Spatiotemporal variations in surface MDA8 O<inline-formula><mml:math id="M73" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M74" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
concentrations</title>
      <p id="d1e990">Figure 2 presents the MDA8 O<inline-formula><mml:math id="M75" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and daily average NO<inline-formula><mml:math id="M76" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations for the first 5 months of 2021–2022 at the 19 sites in Shanghai. In April–May 2022, the concentrations of NO<inline-formula><mml:math id="M77" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>, derived largely from fossil-fuel combustion, decreased by 49 % year-on-year, but the average MDA8 O<inline-formula><mml:math id="M78" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations increased by 12.5 %. (In contrast, PM<inline-formula><mml:math id="M79" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2.5</mml:mn></mml:msub></mml:math></inline-formula> concentrations fell by 30.3 % in Shanghai; Fig. S2b.) The MDA8 O<inline-formula><mml:math id="M80" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations exceeded 160 <inline-formula><mml:math id="M81" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, which is
China's Ambient Air Quality Standard for O<inline-formula><mml:math id="M82" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>, at 1 or more of the 19
sites on 21 d in April–May 2022, with the highest value being 200 <inline-formula><mml:math id="M83" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. The average <inline-formula><mml:math id="M84" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M85" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula>) mixing ratio
in April–May 2022 also increased by 2.2 % during the LCD compared with
the same period in 2021 (Fig. S2a). These observations indicate that there
was significant ground-level O<inline-formula><mml:math id="M86" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution in Shanghai during the 2022
LCD, despite the drastic reductions in human activity. The decrease in
NO<inline-formula><mml:math id="M87" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations (49 %) during the 2022 LCD was larger than the
NO<inline-formula><mml:math id="M88" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> decrease during the full-scale LCD phase in 2020 (23 January–12 February), when the average NO<inline-formula><mml:math id="M89" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentration decreased by 30.5 % from the corresponding period in 2019 (Fig. S3b). During the 2020 LCD, the average MDA8 O<inline-formula><mml:math id="M90" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations in Shanghai increased by 13.8 % but remained far below the ambient O<inline-formula><mml:math id="M91" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration standard (Fig. S3a).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e1183">Temporal variations in surface-level maximum daily 8 h average
(MDA8) O<inline-formula><mml:math id="M92" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> <bold>(a)</bold> and NO<inline-formula><mml:math id="M93" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> <bold>(b)</bold> concentrations during the 2022 pre-lockdown (LCD) (1 January to 27 March) and LCD periods (28 March to 31 May) compared with the corresponding periods in 2021. The concentrations are averages from 19 sites in Shanghai. The trend lines represent prior 2-week moving averages. The insert figures show the monthly average concentrations (bars and values indicated by numbers) and standard deviations (error bars). The red background represents the 2022 LCD in Shanghai (SH LCD 2022: 28 March to 31 May). The <inline-formula><mml:math id="M94" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula>-axis labels represent the first day of each month.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f02.png"/>

        </fig>

      <p id="d1e1223">Figure 3a–c show the spatial distribution of the MDA8 O<inline-formula><mml:math id="M95" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
concentrations in mainland China and the YRD region, which consists of
Shanghai and three neighbouring provinces (Jiangsu, JS; Anhui, AH; and
Zhejiang, ZJ), and Shanghai during the 2022 LCD, respectively. It can be
seen that elevated O<inline-formula><mml:math id="M96" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations were observed at most sites in JS,
in the southern part of ZJ and in the eastern part of AH. These provinces
are known to have close economic ties to Shanghai.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e1247">Spatial distribution of surface maximum daily 8 h average (MDA8) O<inline-formula><mml:math id="M97" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations in 2022 and changes in the same compared with 2021
across all of mainland China <bold>(a, d)</bold>, in the Yangtze River Delta region <bold>(b, e)</bold> and in Shanghai <bold>(c, f)</bold> from 28 March to 31 May 2022. LCD: lockdown.</p></caption>
          <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f03.png"/>

        </fig>

      <p id="d1e1274">The increase in MDA8 O<inline-formula><mml:math id="M98" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations during the 2022 LCD was not
restricted to Shanghai. Figure 3d–f show the spatial distribution of
changes in MDA8 O<inline-formula><mml:math id="M99" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations from 2021 to 2022 at the national,
regional and city scales, respectively. The MDA8 O<inline-formula><mml:math id="M100" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations
clearly increased in central and eastern regions but decreased in
south-western, north-western and north-eastern regions (Fig. 3d). The YRD
region recorded one of the greatest increases in MDA8 O<inline-formula><mml:math id="M101" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations
(17.4 <inline-formula><mml:math id="M102" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) during the 2022 LCD (Fig. 3e). Within Shanghai, the year-on-year increase in MDA8 O<inline-formula><mml:math id="M103" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations decreased from urban to semi-rural areas, with the largest increase recorded in the Putuo district
in the city centre (32.9 <inline-formula><mml:math id="M104" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">g</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) (Fig. 3f).</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><?xmltex \opttitle{TROPOMI-based HCHO and NO${}_{{2}}$ concentrations}?><title>TROPOMI-based HCHO and NO<inline-formula><mml:math id="M105" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations</title>
      <p id="d1e1379">Figure 4 depicts the spatial distributions of TROPOMI-based tropospheric
column concentrations of HCHO and NO<inline-formula><mml:math id="M106" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and the <inline-formula><mml:math id="M107" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> column
ratios in the YRD region. During the 2022 LCD and compared with the same
period in 2021, the column concentrations of HCHO, derived from both direct
emissions and degradation of anthropogenic and natural VOCs, decreased by 10.8 % (Fig. 4a), and the NO<inline-formula><mml:math id="M108" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> column
concentrations decreased by 25.1 % (Fig. 4b). The magnitudes of the
reductions in HCHO and NO<inline-formula><mml:math id="M109" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> column concentrations had similar spatial
distributions, with the largest reductions observed in the region's major
cities (Shanghai, Suzhou, Nanjing and Hangzhou). This indicated that the
reductions in both the NO<inline-formula><mml:math id="M110" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and HCHO column concentrations were related
to decreases in anthropogenic activity during the 2022 LCD. Due to a larger
decrease in NO<inline-formula><mml:math id="M111" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations than in HCHO concentrations, the average
<inline-formula><mml:math id="M112" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio increased from 2.57 in 2021 to 2.96 in 2022 in the YRD
region (Fig. 4c). In Shanghai, the HCHO and NO<inline-formula><mml:math id="M113" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> column concentrations
decreased by 19.4 % and 49.2 %, respectively, during the 2022 LCD (see Sect. 3.3.2 for a detailed discussion). In comparison, the TROPOMI-based
HCHO and NO<inline-formula><mml:math id="M114" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> column concentrations in February 2020 showed 17 % and
38 % decreases, respectively, in the YRD region compared with the same
month in 2019 (Stavrakou et al., 2021). The much larger reduction in NO<inline-formula><mml:math id="M115" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations than in HCHO concentrations during the 2022 LCD is attributable to the fact that <inline-formula><mml:math id="M116" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is mainly emitted by transportation activities (which exhibited the greatest decrease during the 2022 LCD) and by power generation, whereas VOCs are derived from more diverse sources. In Shanghai, the main VOC sources are vehicular exhaust; evaporation of fuels, paints and solvents; petrochemical industries; liquefied petroleum gas; and biogenic sources (Lin et al., 2020; Han et al., 2022).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e1498">Spatial distribution of the TROPOspheric Monitoring Instrument-based tropospheric column concentrations of HCHO <bold>(a)</bold> and NO<inline-formula><mml:math id="M117" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> <bold>(b)</bold> and the <inline-formula><mml:math id="M118" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio <bold>(c)</bold> in the Yangtze River Delta region during the 2022 lockdown (upper row) and compared with the same period in 2021 (lower row).</p></caption>
          <?xmltex \igopts{width=426.791339pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f04.png"/>

        </fig>

<?xmltex \hack{\newpage}?>
</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><?xmltex \opttitle{Cause(s) of high O${}_{{3}}$ concentrations during the 2022 LCD}?><title>Cause(s) of high O<inline-formula><mml:math id="M119" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations during the 2022 LCD</title>
<sec id="Ch1.S3.SS3.SSS1">
  <label>3.3.1</label><?xmltex \opttitle{Effects of meteorological conditions on O${}_{{3}}$ pollution in Shanghai}?><title>Effects of meteorological conditions on O<inline-formula><mml:math id="M120" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution in Shanghai</title>
      <p id="d1e1577">A large body of literature has indicated that meteorological conditions can significantly affect O<inline-formula><mml:math id="M121" display="inline"><mml:msub><mml:mi/><mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/></mml:mrow></mml:msub></mml:math></inline-formula>concentrations by altering emissions, chemical reaction rates, and distribution and removal processes (e.g. Lu et al., 2019; Liu and Wang, 2020; Liu et al., 2021; Jacob and Winner, 2009; Lin et al., 2008; He et al., 2017). To gain insights into the weather
conditions during the 2022 LCD period, we compared several meteorological
parameters recorded at surfaces in Shanghai (temperature, RH, and wind speed
and direction) (Fig. 5) and the ERA5 reanalysis data for large regions (Fig. 6). The results indicate that during the 2022 LCD, the average surface air temperature and RH decreased compared with the same period in 2021. That is, the mean temperature was 18.4 <inline-formula><mml:math id="M122" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>C in 2022 versus 19.9 <inline-formula><mml:math id="M123" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>C in 2021, and the mean RH was 71.4 % in 2022 versus 74.2 % in 2021
(Fig. 5a–b). The ERA5 reanalysis data revealed there was a decrease in the
surface (2 m) temperature in Shanghai, whereas there was an obvious increase
in the 2 m temperature in the northern part of the YRD region and a large
decrease in the 2 m temperature in the southern part of the YRD region (Fig. 6). The decrease in mean temperature in Shanghai during the 2022
LCD may have slowed O<inline-formula><mml:math id="M124" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> production by reducing chemical reaction rates
and biogenic emissions. The ERA5 reanalysis data also revealed that during
the 2022 LCD there were insignificant changes in cloud cover, downward UV
radiation, boundary layer heights and total precipitation in Shanghai but
considerable changes in these parameters in the surrounding areas (Fig. 6).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e1620">A comparison of average temperature <bold>(a)</bold> and relative humidity <bold>(b)</bold> in April and May of 2021 and 2022. Wind rose plots for the 2022 lockdown period <bold>(c)</bold> and the same period in 2021 <bold>(d)</bold>. The data are surface observations.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f05.png"/>

          </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e1644">Percentage change in the average meteorological parameters of European Centre for Medium-Range Weather Forecast reanalysis v5 data for the
Yangtze River Delta and its neighbouring regions. The 2 m temperature (t2m) <bold>(a)</bold>, downward ultraviolet (UV) radiation at the surface (uvb) <bold>(b)</bold>, total precipitation (tp) <bold>(c)</bold>, relative humidity at 1000 hPa (r) <bold>(d)</bold>, total cloud cover (tcc) <bold>(e)</bold> and boundary layer height (blh) <bold>(f)</bold>.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f06.png"/>

          </fig>

      <p id="d1e1672">We also assessed whether there was a significant change in surface airflow
in Shanghai during the 2022 LCD compared with the preceding year. An
examination of surface winds in Shanghai showed that during the 2022 LCD,
predominant surface winds were from the north-east–south-east sectors (Fig. 5c–d), which is consistent with the 24 h calculated back trajectories (Fig. S4). This indicates that for the majority of the 2022 LCD, Shanghai was
upwind of other cities in the YRD region. Compared with the same period in
2021, during the 2022 LCD there was an increase in the occurrence of
northerly winds and a decrease in the occurrence of westerly winds. To check
for transport of O<inline-formula><mml:math id="M125" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> from high-O<inline-formula><mml:math id="M126" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> areas in the north-west direction,
we examined surface wind flows during the 21 O<inline-formula><mml:math id="M127" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> exceedance days. Both
surface wind flows and back trajectories indicated that during these days
air mainly came from the north-east–east–south-east directions (Fig. 7),
indicating that air from other YRD cities contributed little to the
high-O<inline-formula><mml:math id="M128" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> days in Shanghai during the 2022 LCD.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e1713"><bold>(a)</bold> The 24 h back trajectories at 1 h intervals at a height of 500 m and <bold>(b)</bold> surface wind rose plot for the 21 O<inline-formula><mml:math id="M129" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> exceedance days during the 2022 lockdown in Shanghai. The inserted percentages represent the percentages of trajectory numbers of each classification in the whole trajectories.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f07.png"/>

          </fig>

      <p id="d1e1736">The above results suggest that the increase in O<inline-formula><mml:math id="M130" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations in
Shanghai during the 2022 LCD were not due to changes in meteorological
conditions but were a result of local chemical production.</p>
</sec>
<sec id="Ch1.S3.SS3.SSS2">
  <label>3.3.2</label><?xmltex \opttitle{Effect of the changes in O${}_{{3}}$ formation regimes in Shanghai}?><title>Effect of the changes in O<inline-formula><mml:math id="M131" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> formation regimes in Shanghai</title>
      <p id="d1e1766">The photochemical production of O<inline-formula><mml:math id="M132" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> is controlled by the non-linear
chemistry of <inline-formula><mml:math id="M133" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (NO and NO<inline-formula><mml:math id="M134" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>) and VOCs
(NRC, 1992). It is well known that in many cities, O<inline-formula><mml:math id="M135" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations decrease as VOC emissions decrease but increase as <inline-formula><mml:math id="M136" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emissions decrease (e.g. Wang et al., 2022). The literature has shown that Shanghai largely operates within a VOC-limited regime (e.g. Lin et al., 2020). We found observational evidence – the <inline-formula><mml:math id="M137" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios and the relationship between O<inline-formula><mml:math id="M138" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M139" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations – that shows that the city remained in a VOC-limited regime before the 2022 LCD (both in the earlier months of 2022 and in April–May of 2021) but may have transitioned near a <inline-formula><mml:math id="M140" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>–VOC-co-limited regime during the 2022 LCD. The <inline-formula><mml:math id="M141" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio has been used as a proxy for O<inline-formula><mml:math id="M142" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> formation regimes, with low ratios indicating VOC-limited conditions, high ratios indicating <inline-formula><mml:math id="M143" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-limited conditions and intermediate values indicating a co-limited regime. Figure 8 shows the temporal variations in city-average <inline-formula><mml:math id="M144" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios in January–May of 2021 and 2022 (Fig. 8a) and the spatial variation in the ratios in Shanghai (Fig. 8b). It indicates that the ratios were comparable (0.56 versus 0.58) in the pre-2022-LCD months of 2021 and 2022 but significantly increased during the 2022 LCD (from 1.11 to 1.68) (Figs. 8a and S5). Moreover, the ratios were higher in the southern part than the northern part of Shanghai, which houses the major urban districts (Fig. 8b).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><?xmltex \currentcnt{8}?><?xmltex \def\figurename{Figure}?><label>Figure 8</label><caption><p id="d1e1916">Temporal variations in the city-average <inline-formula><mml:math id="M145" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio from 1 January to 31 May of 2021 and 2022 <bold>(a)</bold>. Spatial variations in the <inline-formula><mml:math id="M146" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio in Shanghai and its surrounding regions during the 2022 lockdown <bold>(b)</bold>. The trend lines in panel <bold>(a)</bold> represent the moving average by 2 weeks. The dashed vertical red line represents the lockdown starting date (27 March), and the insert shows the monthly average <inline-formula><mml:math id="M147" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios with standard deviations.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f08.png"/>

          </fig>

      <p id="d1e1980">Previous analysis of the historical Ozone Monitoring Instrument (OMI) <inline-formula><mml:math id="M148" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios in Shanghai
indicated a general rising trend in the ratios with values ranging from
0.5–1.5 in 2005–2019 in warm seasons (April–September) (Itahashi et al., 2022; Li et al., 2021; Lee et al., 2022). For April and May, the
months when the 2022 Shanghai LCD took place, the <inline-formula><mml:math id="M149" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios
ranging from 0.73 to 1.36 were in 9 out of 10 years during 2010–2019, with a
higher ratio (1.61) for the year 2014 (Li et al., 2021). This shows that the <inline-formula><mml:math id="M150" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio during LCD 2022 (1.68) was high compared with that of the same months in the past decade, resulting from the sharply reduced NO<inline-formula><mml:math id="M151" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> column concentrations during the LCD. Several other megacities in East Asia have also seen increasing <inline-formula><mml:math id="M152" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios during 2015–2019 (Itahashi et al., 2022; Lee et al., 2022).</p>
      <p id="d1e2053">To determine the regime transition threshold, we adopted an observation-based method similar to that which has been used by previous researchers (Jin et al., 2020; Wang et al., 2021; Schroeder et al., 2022): we plotted the
city-average MDA8 O<inline-formula><mml:math id="M153" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations against the <inline-formula><mml:math id="M154" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio for the first 5 months of 2021 and 2022 (Fig. 9). The peak O<inline-formula><mml:math id="M155" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations increased as the <inline-formula><mml:math id="M156" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio increased and plateaued at approximately 2, indicating that a <inline-formula><mml:math id="M157" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio of 2 was the threshold for transition from a VOC-limited to a co-limited regime. This value is similar to that determined (2.3) for other major Chinese cities
(Wang et al., 2021); however, it is less than that determined (<inline-formula><mml:math id="M158" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula>) for several US cities (Jin et al., 2020) and greater than that derived from model simulations (Duncan et al., 2010; Li et al., 2021). The city-averaged <inline-formula><mml:math id="M159" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio was greater than 2 on 15 d during the 2022 LCD but on just 2 d in 2021 (see Fig. 9). Moreover, a spatial analysis shows that during the 2022 LCD, the southern part of Shanghai was in a VOC–<inline-formula><mml:math id="M160" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-co-limited regime (with a <inline-formula><mml:math id="M161" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio <inline-formula><mml:math id="M162" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>), whereas the city centre in the northern part remained in the VOC-limited regime (Fig. 8b).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><?xmltex \currentcnt{9}?><?xmltex \def\figurename{Figure}?><label>Figure 9</label><caption><p id="d1e2183">Scatterplot of Shanghai's average maximum daily 8 h (MDA8)
O<inline-formula><mml:math id="M163" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations and <inline-formula><mml:math id="M164" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratios in January–May of 2021
(blue dots) and 2022 (red dots). The data points recorded during the
lockdown periods are labelled with red crosses.</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f09.png"/>

          </fig>

      <p id="d1e2216">The relationship between surface O<inline-formula><mml:math id="M165" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and NO<inline-formula><mml:math id="M166" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations
supports the inference made based on satellite-derived <inline-formula><mml:math id="M167" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio
data. It is known that O<inline-formula><mml:math id="M168" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations are negatively correlated with
<inline-formula><mml:math id="M169" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M170" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>y</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> or <inline-formula><mml:math id="M171" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>z</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> concentrations (<inline-formula><mml:math id="M172" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>y</mml:mi></mml:msub></mml:mrow><mml:mo>=</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow><mml:mo>+</mml:mo></mml:mrow></mml:math></inline-formula> oxidation products of <inline-formula><mml:math id="M173" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M174" display="inline"><mml:mrow class="chem"><mml:mo>[</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>z</mml:mi></mml:msub><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula>) under a <inline-formula><mml:math id="M175" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-titrated condition; this relationship is slightly positive (with small <inline-formula><mml:math id="M176" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> ratios) in a VOC-limited regime and very positive (with large <inline-formula><mml:math id="M177" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> ratios) in a <inline-formula><mml:math id="M178" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-limited
regime. For example, previous studies have suggested that an afternoon
<inline-formula><mml:math id="M179" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>z</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> ratio (ppb <inline-formula><mml:math id="M180" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula> ppb) less than 4 corresponds to a VOC-limited regime, an afternoon <inline-formula><mml:math id="M181" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>z</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> ratio greater than 7 corresponds to a <inline-formula><mml:math id="M182" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-limited regime, and an afternoon <inline-formula><mml:math id="M183" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>z</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> of 4–7 corresponds to a transition regime (Wang et al., 2017). Only NO<inline-formula><mml:math id="M184" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and <inline-formula><mml:math id="M185" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (not other forms of reactive nitrogen) are measured by most regular air-monitoring networks, including the China Environmental Monitoring Network used in this study. Figure 10 shows the scatterplot of the MDA8 O<inline-formula><mml:math id="M186" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and daily average NO<inline-formula><mml:math id="M187" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations at three types of sites in Shanghai: the city centre (12 sites), the city perimeter (4 sites) and the semi-rural areas (2 sites). The VOC-limited regime at the city centre sites (with an average <inline-formula><mml:math id="M188" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio of 1.43) had the smallest <inline-formula><mml:math id="M189" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> slope (3.4), and that in the transition regime sites (with a <inline-formula><mml:math id="M190" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio of 2.27) had the largest <inline-formula><mml:math id="M191" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> slope (5). In comparison, in 2021, the peak O<inline-formula><mml:math id="M192" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration had either a very weak or no correlation with NO<inline-formula><mml:math id="M193" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations, indicative of a typical VOC-limited regime. (The type D site had small positive <inline-formula><mml:math id="M194" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> slopes in both years (0.89–1.17), with high NO<inline-formula><mml:math id="M195" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> during the 2022 LCD possibly from the ship emissions in the Yangtze River Estuary; Fig. S6.)</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10" specific-use="star"><?xmltex \currentcnt{10}?><?xmltex \def\figurename{Figure}?><label>Figure 10</label><caption><p id="d1e2648">Scatterplots of the surface maximum daily 8 h average (MDA8)
O<inline-formula><mml:math id="M196" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations versus surface daily NO<inline-formula><mml:math id="M197" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations and
their linear regressions (straight lines) during the 2022 lockdown <bold>(a)</bold> and the same period in 2021 <bold>(b)</bold> for three types of sites.</p></caption>
            <?xmltex \igopts{width=426.791339pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/14455/2022/acp-22-14455-2022-f10.png"/>

          </fig>

      <p id="d1e2681">The above results suggest that the increased O<inline-formula><mml:math id="M198" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations observed
during the 2022 LCD were mainly due to increased O<inline-formula><mml:math id="M199" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> production, which
resulted from a larger reduction in <inline-formula><mml:math id="M200" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emissions than in VOC emissions
under a VOC-limited condition. Additionally, the decrease in particulate
emissions, which reduces the uptake of radicals and O<inline-formula><mml:math id="M201" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> and increases
radiation, could have increased O<inline-formula><mml:math id="M202" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations. Previous model
simulations of the 2020 LCD in central China, which saw similar decreases in emissions (i.e. <inline-formula><mml:math id="M203" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>: <inline-formula><mml:math id="M204" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> %; PM: <inline-formula><mml:math id="M205" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">30</mml:mn></mml:mrow></mml:math></inline-formula> %), showed that the decrease in <inline-formula><mml:math id="M206" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emissions made a much larger
contribution than the decrease in PM emissions to the increase in O<inline-formula><mml:math id="M207" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
concentrations (Liu et al., 2021). We believe that this also occurred during the 2022 LCD; i.e. the O<inline-formula><mml:math id="M208" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentration increase was mainly due to enhanced O<inline-formula><mml:math id="M209" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> production, which occurred as a result of a large reduction in <inline-formula><mml:math id="M210" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emissions. The O<inline-formula><mml:math id="M211" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> formation regime during the 2022 LCD remained VOC-limited in urban areas but entered co-limiting conditions outside the city centre.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S4" sec-type="conclusions">
  <label>4</label><title>Summary and implications</title>
      <p id="d1e2832">This study analysed the causes of frequent ground-level O<inline-formula><mml:math id="M212" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution during the 2022 LCD (April–May 2022) in Shanghai and assessed the increases in O<inline-formula><mml:math id="M213" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations compared with the same periods in previous years using ground and satellite-based observations. We found that despite large reductions in the activities of transportation sectors and industries during the 2022 LCD, frequent exceedances of the O<inline-formula><mml:math id="M214" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> air quality standard
(<inline-formula><mml:math id="M215" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">30</mml:mn></mml:mrow></mml:math></inline-formula> % days) were observed at ground level. Moreover, the
O<inline-formula><mml:math id="M216" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations were increased during the 2022 LCD compared with the same period in the preceding year. This increase resulted from a large
reduction in <inline-formula><mml:math id="M217" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> emissions (<inline-formula><mml:math id="M218" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> % from surface and satellite-based measurements) and a small reduction in VOCs (19 % in HCHO column concentrations) within Shanghai. In contrast, meteorology and outside influences had insignificant effects on O<inline-formula><mml:math id="M219" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> concentrations during the 2022 LCD. Moreover, O<inline-formula><mml:math id="M220" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> formation during the 2022 LCD remained in the VOC-limited regime at most urban and suburban sites but transitioned to a VOC–<inline-formula><mml:math id="M221" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-co-limited regime in semi-rural areas.</p>
      <p id="d1e2932">Our findings on the O<inline-formula><mml:math id="M222" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> response to the 2022 LCD have implications for
mitigating summer O<inline-formula><mml:math id="M223" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution, which has become the predominant
air-pollution problem during warm seasons in China. O<inline-formula><mml:math id="M224" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution is
also a persistent environmental hazard in the US and Europe even after a few decades of research and control (e.g. Tao et al., 2022; Derwent and Parrish, 2022). Similar to Shanghai, many of the world's cities, such as Los Angeles and New York, are still in VOC-limited regimes (Jin et al., 2020; Tao et al., 2022). Our results show that drastically
decreasing emissions from conventional fossil-fuel-powered transportation
sectors during the 2022 LCD can lead to increased and elevated O<inline-formula><mml:math id="M225" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
concentrations in VOC-limited urban areas. China is aiming to have its
carbon emissions peak by 2030 and to achieve carbon neutrality by 2060, and other countries are also committing to drastically reducing their carbon
emissions. This will necessitate the rapid uptake of electric vehicles in
many cities. However, although large-scale adoption of electric vehicles
will greatly improve overall air quality, VOC emissions from other sectors
will need to be decreased at the same time to prevent increases in O<inline-formula><mml:math id="M226" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula>
concentrations from the reductions in <inline-formula><mml:math id="M227" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (and particulate) emissions in the early stages of phase-out of conventional vehicles. Over time, the wide application and acceptance of renewable energy in transportation and energy production will help cities reach the <inline-formula><mml:math id="M228" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-limited formation regime, alleviate ground-level O<inline-formula><mml:math id="M229" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution and achieve carbon-reduction targets. The aggravated O<inline-formula><mml:math id="M230" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:math></inline-formula> pollution during the 2022 Shanghai LCD after large reductions in transportation emissions suggests that it may take a considerably long time for some cities to reach a <inline-formula><mml:math id="M231" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-limited regime.</p>
</sec>

      
      </body>
    <back><notes notes-type="codedataavailability"><title>Code and data availability</title>

      <p id="d1e3036">The code and data used in this study are available upon request from Tao Wang (tao.wang@polyu.edu.hk).</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e3039">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-22-14455-2022-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-22-14455-2022-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e3048">TW initiated the research and designed the framework of data analysis. YT processed the data and made the figures. TW and YT analysed the results and wrote the paper.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e3054">At least one of the (co-)authors is a member of the editorial board of <italic>Atmospheric Chemistry and Physics</italic>. The peer-review process was guided by an independent editor, and the authors also have no other competing interests to declare.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d1e3063">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e3069">We thank Shanshan Wang at Fudan University for
providing the OMI <inline-formula><mml:math id="M232" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">HCHO</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ratio data in Shanghai during 2010–2019.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e3089">This research has been supported by the Hong Kong Research Grants Council (grant no. T24-504/17-N) and the National Natural Science Foundation of China (grant no. 91844301).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e3096">This paper was edited by Jianzhong Ma and reviewed by Hongbo Fu and one anonymous referee.</p>
  </notes><ref-list>
    <title>References</title>

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