Rethinking the role of transport and photochemistry in regional ozone
pollution: Insights from ozone mass and concentration budgets
Abstract
Understanding the role of transport and photochemistry is essential to
alleviate ambient ozone pollution. However, ozone budget and source
apportionment studies often report conflicting conclusions — Local
photochemistry is the main cause of ozone pollution based on the
analyses of the former, while contrary, non-local ozone transported to
the region accounts for the majority in the latter results. In order to
explore its potential causes, we calculated the contributions of both
processes to the variations of mean ozone concentration and total ozone
mass (the corresponding budgets are noted as ozone concentration and
mass budget, respectively) within the atmospheric boundary layer (ABL)
of the Pearl River Delta (PRD), China, based on the modelling results of
WRF-CMAQ. Quantified results show that photochemistry drives the rapid
increase of ozone concentrations in the daytime, whereas transport,
especially the vertical exchange near the ABL top, controls the ozone
mass budget. The changes in transport contributions in ozone budgets
indicate the influences of the ABL diurnal cycle and regional wind
fields, including prevailing winds and local circulations (sea breezes),
on regional ozone pollution. Though transport in our simulations had a
relatively limited effect on ozone concentration, its high contribution
to ozone mass increase in the morning determined that most ozone in the
PRD emanated from the outer regions. Consequently, the role of transport
and photochemistry in ozone pollution may differ, depending on which of
the two budgets is concerned. For future studies targeting ozone and
other pollutants with moderately long atmospheric lifetimes, we suggest
that attention should be paid to budget-type selections.