Particle-bound mercury (PBM) records the oxidation of elemental mercury, of which the main oxidation pathways (Br•/Cl•/OH•/O 3 ) remain unclear, especially in the Southern Hemisphere. Here, we present latitudinal covariations of Hg and Sisotopic anomalies in cross-hemispheric marine aerosols that evidence an equator-to-poleward transition of Hg oxidants from OH•/O 3 in tropics to Br•/Cl• in polar regions highlighting thus the presence of distinct oxidation processes producing PBM. The correlations between Hg, S and O-isotopic compositions measured in PBM, sulfates and nitrates respectively within the aerosols highlight the implication of common oxidants in their formations at different latitudes. Our results open a new window to better quantify the present-day atmospheric Hg, S and N budgets and to evaluate the influences of aerosols on climate and ecosystems once the isotopic fractionations associated with each process have been determined.
The mechanisms triggering the large variations in the mercury (Hg) multiple isotopic compositions of atmospheric particle-bound Hg worldwide still remain unclear. The comparison of Hg isotopic compositions in aerosols collected in urban and rural areas may help distinguish the effects of natural processes from those of anthropogenic inputs. We thus investigated the Hg isotopic compositions of PM10 aerosols collected seasonally during 2015 at two monitoring stations on Montreal Island, one located downtown and the other in its westernmost subrural part, barely impacted by the city anthropogenic emissions. Our results show that, while Hg isotopic compositions present no seasonality at the urban station, possibly due to constant anthropogenic emissions, the subrural samples display clear seasonal variations, with higher Δ199Hg and Δ200Hg values (up to 0.77 and 0.12‰, respectively) during summer and close to 0‰ during the rest of the year, that cannot solely be explained by anthropogenic primary emissions. Besides, Δ200Hg measured in the subrural aerosols display a positive correlation with O3 suggesting the implication of secondary processes involving ozone. We propose that the significant summer shift in the multiple Hg isotopic compositions may reflect a transition in the corresponding Hg0 oxidation pathway, from halogens-triggered to ozone-dominated reactions. Still, this hypothesis needs to be further tested. Nevertheless, it demonstrates that Hg isotopes are effective at characterizing secondary processes that control its atmospheric budget, even at a local scale (i.e., urban vs subrural) and could thus be used to better constrain its atmospheric chemistry in various environments.
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