Isotopic Evidence Suggests a Predominant Anthropogenic Contribution to Particulate Sulfate in the Coastal Marine Boundary Layer
ID:81
Oral Presentation
2027-01-14 14:30 (China Standard Time)
Session:Session 1 - Coastal ecosystem by anthropogenic activities and climate changes
Abstract
Sulfate (SO42-), plays a key role in the formation, growth, and chemical properties of aerosol particles and cloud droplets in marine boundary layer, with profound implications for climate and air quality. Despite this, the formation pathways and emission sources of particulate sulfate under a mixed marine–continental environment remain highly unconstrained. Here, year-round sulfur isotopic composition of PM2.5 sulfate was measured over, together with that of SO2 in summer and winter. During the observation period, sulfate accounted for 20–70% of the total water-soluble inorganic ions in PM2.5, highlighting its substantial contribution to coastal particulate pollution. The δ34S–SO42- values were found higher in spring and summer (9.0±2.3‰) than in autumn and winter (6.6±2.2‰), together with the higher δ34S–SO2 values observed in summer than that in winter. The corresponding sulfur isotope fractionation between gas-phase SO2 and particulate SO42- were further determined for the pathway resolution. Results suggest photochemically driven oxidation by H2O2/O3 and OH collectively dominated secondary sulfate formation, contributing approximately 50% in all four seasons. By contrast, the contributions of transition-metal-ion (TMI) catalyzed oxidation and HOCl oxidation exhibited pronounced seasonal variability, with lower contributions in spring and summer than in autumn and winter. This pattern suggests an enhanced influence of polluted continental air masses from inland northern China during the colder seasons. Source apportionment results derived from the isotopic composition of sulfur emission showed that vehicle emissions (36.5–46.9%) and coal combustion (33.5–40.8%) were the principal sources of ambient sulfur across the four seasons. Ship emissions contributed 7.5–13.0%, whereas marine biogenic dimethyl sulfide (DMS) made a comparatively small contribution, reaching a maximum of 9.8% in summer and a minimum of 3.6% in winter. Thus, despite the frequent influence of marine air masses, particulate sulfate in this coastal city was predominantly derived from local and regionally transported anthropogenic emissions, while marine sulfur sources played a relatively limited role. These findings demonstrate the importance of controlling vehicle- and coal-related emissions for mitigating particulate sulfate pollution in coastal regions in eastern China.
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Important Dates
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Jan 30
2026
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Mar 31
2026
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Apr 30
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2026
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Sep 15
2026
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Oct 15
2026
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Jan 12–15
2027
XMAS 2027
