Abstract. Severe surface ozone pollution over major Chinese cities has become an
emerging air quality concern, raising a new challenge for emission control
measures in China. In this study, we explore the source contributions to
surface daily maximum 8 h average (MDA8) ozone over China in 2016 and 2017,
the 2 years with the highest surface ozone averaged over Chinese cities in
record. We estimate the contributions of anthropogenic, background, and
individual natural sources to surface ozone over China using the GEOS-Chem
chemical transport model at 0.25∘×0.3125∘
horizontal resolution with the most up-to-date Chinese anthropogenic
emission inventory. Model results are evaluated with concurrent surface
ozone measurements at 169 cities over China and show generally good agreement.
We find that background ozone (defined as ozone that would be present in
the absence of all Chinese anthropogenic emissions) accounts for 90 %
(49.4 ppbv) of the national March–April mean surface MDA8 ozone over China
and 80 % (44.5 ppbv) for May–August. It includes large contributions from
natural sources (80 % in March–April and 72 % in May–August). Among
them, biogenic volatile organic compound (BVOC) emissions enhance MDA8
ozone by more than 15 ppbv in eastern China during July–August, while
lightning NOx emissions and ozone transport from the stratosphere both
lead to ozone enhancements of over 20 ppbv in western China during
March–April. Over major Chinese city clusters, domestic anthropogenic
sources account for about 30 % of the May–August mean surface MDA8 ozone
and reach 39–73 ppbv (38 %–69 %) for days with simulated MDA8 ozone
> 100 ppbv in the North China Plain, Fenwei Plain, Yangtze
River Delta, and Pearl River Delta city clusters. These high ozone episodes
are usually associated with high temperatures, which induce large BVOC
emissions and enhance ozone chemical production. Our results indicate that
there would be no days with MDA8 ozone > 80 ppbv in these major
Chinese cities in the absence of domestic anthropogenic emissions. We find
that the 2017 ozone increases relative to 2016 are largely due to higher
background ozone driven by hotter and drier weather conditions, while
changes in domestic anthropogenic emissions alone would have led to ozone
decreases in 2017. Meteorological conditions in 2017 favor natural source
contributions (particularly soil NOx and BVOC ozone enhancements) and
ozone chemical production, increase the thermal decomposition of peroxyacetyl
nitrate (PAN), and further decrease ozone dry deposition velocity. More
stringent emission control measures are thus required to offset the adverse
effects of unfavorable meteorology, such as high temperature, on surface ozone
air quality.