Abstract
Atmospheric nitrate deposition resulting from anthropogenic activities
negatively affects human and environmental health. Identifying deposited
nitrate that is produced locally vs. that originating from long-distance
transport would help inform efforts to mitigate such impacts. However,
distinguishing the relative transport distances of atmospheric nitrate in
urban areas remains a major challenge since it may be produced locally and/or
be transported from upwind regions. To address this uncertainty we assessed
spatiotemporal variation in monthly weighted-average Δ17O and
δ15N values of wet and dry nitrate deposition during one year at
urban and rural sites along the western coast of the northern Japanese island
of Hokkaido, downwind of the East Asian continent. Δ17O values of
nitrate in wet deposition at the urban site mirrored those of wet and dry
deposition at the rural site, ranging between ∼ +23 and
+31 ‰ with higher values during winter and lower values in summer,
which suggests the greater relative importance of oxidation of NO2 by
O3 during winter and OH during summer. In contrast, Δ17O
values of nitrate in dry deposition at the urban site were lower
(+19 – +25 ‰) and displayed less distinct seasonal variation.
Furthermore, the difference between δ15N values of nitrate in wet
and dry nitrate deposition was, on average, 3 ‰ greater at the urban
than rural site, and Δ17O and δ15N values were correlated
for both forms of deposition at both sites with the exception of dry
deposition at the urban site. These results suggest that, relative to nitrate
in wet and dry deposition in rural environments and wet deposition in urban
environments, nitrate in dry deposition in urban environments forms from
relatively greater oxidation of NO by peroxy radicals and/or oxidation of
NO2 by OH. Given greater concentrations of peroxy radicals and OH in
cities, these results imply that dry nitrate deposition results from local
NOx emissions more so than wet deposition, which is transported longer
distances. These results illustrate the value of stable isotope data for
distinguishing the transport distances and reaction pathways of atmospheric
nitrate pollution.
Citation
ID:
196599
Ref Key:
nelson2018atmospherictriple