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Hong-Hai Zhang, Gui-Peng Yang, Chun-Ying Liu, and Lu-Ping Su

Abstract

The total suspended particulate (TSP) samples over the Yellow Sea and the East China Sea were collected to determine the major compositions of water-soluble ionic species during two cruises in autumn 2007. The aerosol compositions exhibited an obvious regional variation between the two cruises, with higher concentrations (except Na+ and Mg2+) over the northern Yellow Sea during the first cruise. The concentrations of the secondary ions [non–sea salt sulfate (nss-), , and ] were 11 ± 4.9, 3.1 ± 2.1, and 3.7 ± 2.6 μg m−3, respectively, which together contributed over 72% of the total determined ion concentrations. Significant correlations between these secondary ions were found within each sampling period, while nss-K+ and nss-Ca2+ showed strong correlation with each other. The calculated results of equivalent concentrations of anions (nss- and ) and cations ( and Ca2+) showed that the acidic species were mostly neutralized with the alkaline species over the study areas. The mass ratio of nss-/ was 1.4 during the investigation period. In addition, the concentrations of MSA were 0.011 ± 0.044 and 0.0081 ± 0.0047 μg m−3 during the two cruises, respectively. Based on the measured MSA, nss-, and their ratios, the relative biogenic sulfur contribution to the total nss- was estimated to be only 2.0% during the two cruises, further suggesting the major contribution of anthropogenic source to sulfur budget over the marginal seas of China.

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Yan Zhang, Hong-Hai Zhang, Gui-Peng Yang, and Qiu-Lin Liu

Abstract

The total suspended particulate (TSP) samples over the Bohai Sea and the Yellow Sea were collected during two cruises in spring and autumn in 2012. Concentrations of water-soluble ions {Na+, K+, NH4+, Mg2+, Ca2+, Cl, NO3, SO42−, and CH3SO3 [methanesulfonic acid (MSA)]} and trace metals (Al, Pb, Zn, Cd, Cu, and V) were measured. Mass concentrations of TSP samples ranged from 65.2 to 136 μg m−3 in spring and from 15.9 to 70.3 μg m−3 in autumn, with average values of 100 ± 22.4 and 40.2 ± 17.8 μg m−3, respectively. The aerosol was acidic throughout the sampling periods according to calculation of equivalent concentrations of the cations (NH4+, nss-Ca2+, and nss-K+) and anions (nss-SO42− and NO3). Correlation analysis and enrichment factors revealed that the aerosol composition in the coastal marine atmosphere had a feature of a mixture of air masses: that is, crustal, marine, and anthropogenic emissions. Trace metals were enriched by a wide range of 1–103, and enrichment factors for crustal source (EFc) were relatively higher in spring. Species like Cd, Zn, and Pb had an overwhelming contribution from anthropogenic sources. In addition, the concentrations of MSA varied from 0.0075 to 0.17 and from 0.0019 to 0.018 μg m−3 during the spring and autumn cruises, respectively, with means of 0.061 and 0.012 μg m−3, respectively. Based on the observed MSA and nss-SO42− concentrations in spring and autumn, the relative biogenic sulfur contributions to nss-SO42− were estimated to be 8.0% and 3.5% on average, respectively, implying that anthropogenic sources had a dominant contribution to the sulfur budget over the observational area.

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