Filterable and Condensable Particulate Nitrate Emissions from Plumes over North China

Particulate nitrate (NO3–) over North
China is commonly treated as a purely secondary product in chemical
transport models (CTMs), yet persistent low bias suggests a missing
source. Here, we quantified plume primary NO3– (P-NO3–, filterable + condensable)
over North China by integrating a sector-specific emissions framework,
oxygen-isotope constraints, and WRF-CMAQ sensitivity simulations for
January and August 2019. We compiled a China-specific source-profile
database for filterable P-NO3– and constructed
a comprehensive condensable particulate matter (CPM) inventory across
9 anthropogenic sectors. The plume P-NO3– emissions were dominated by the condensable fraction (91.5%) and
industrial and power sources (92.5%). Adding CPM in CMAQ increased
near-surface pNO3– by 0.98 ± 0.48
μg m–3 (10.1 ± 4.8%) in the summer and
0.99 ± 0.45 μg m–3 (4.6 ± 1.7%)
in the winter, improving model performance with the response primarily
expressed as enhanced emissions rather than aerosol chemistry. Similarly,
a Bayesian δ18O model using a low-δ18O plume end member (20.2 ± 7.8‰) yields plume P-NO3– contributions of 13.1 ± 4.0% (summer)
and 4.5 ± 2.0% (winter) and showed that omitting this end member
systematically overestimated NO3– to
the ·OH+NO2 pathway. These findings highlighted CPM-driven
plume P-NO3– as a missing source that
should be explicitly represented in inventories, CTMs, and NO3– mitigation strategies.