Abstract

Atmospheric deposition of long-range transported continental substances from natural and anthropogenic sources affects biogeochemical processes in marine systems. Emissions of sea spray contribute aerosol particles to the marine atmosphere. Despite the importance of continental dispersion and atmospheric processes involving aerosol particles within remote marine atmosphere, knowledge of the sources of various water-soluble ions is limited because of insufficient observations. Concentrations of Total suspended particulates (TSPs) and major inorganic ions (Cl−, Na+, SO42−, Mg2+, Ca2+, K+, NO3−, NH4+), as well as organic nitrogen (ON-N) values, were measured in marine aerosol collected over the western north Pacific (WNP) during a cruise from 3 December 2014 to 13 March 2015. Aerosol samples were analyzed to determine their chemical characteristics and a source apportionment for this region and the continental influence on the open ocean when air masses are from continent in winter. TSP mass concentrations ranged from 14.1 to 136.0 μg/m3 with an average of 44.8 ± 28.1 μg/m3. Concentrations of TSPs and major ions were higher near the coast (close to Qingdao and Xiamen) and lower over the open ocean. The total mass of inorganic ions and organic nitrogen accounted for 51.1% of the total TSP. Cl− had highest concentrations among the major inorganic ions, followed by SO42−, NO3−, Mg2+, Ca2+, K+, and NH4+, respectively. However, Cl− showed a deficit relative to Na+ in most samples, likely related to heterogeneous reactions within the marine atmosphere. Most SO42−, Mg2+, Ca2+, and K+ were from sea salt, while other major ions were from continental sources. The non-sea-salt (nss) fractions of Ca2+, Mg2+ and K+ were derived from continental crust, while nss-SO42− and NO3− were derived from anthropogenic sources. ON had several sources, including reactions of NOx with volatile organic compounds (anthropogenic sources) or NH3 with gaseous hydrocarbons, as well as crustal and marine biogenic sources.

Highlights

  • The long-distance transport of atmospheric aerosol particles from natural and anthropogenic sources affects ocean ecosystems, climate, and atmospheric chemical processes [1,2,3]

  • The highest Total suspended particulates (TSPs) concentration was measured in the Bashi Channel near Xiamen, followed by 3 much lower than those values in winter at Yongxing Island in the South China Sea (158.9 μg/m ) [2]

  • The average TSP concentration over the western North Pacific Ocean (WNP) was and over the Northern Yellow Sea (145.2 μg/m3 ) [1], consistent with their respective aerosol optical thickness (AOT) distributions much lower than those values in winter at Yongxing Island in the South China Sea (158.9 μg/m3) [2]

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Summary

Introduction

The long-distance transport of atmospheric aerosol particles from natural and anthropogenic sources affects ocean ecosystems, climate, and atmospheric chemical processes [1,2,3]. Primary aerosol particles are emitted directly from natural and anthropogenic sources, while secondary aerosol particles form from condensable atmospheric gases [2]. In the remote marine atmosphere, ions from sea salt make significant contributions to the aerosol mass of Na+ , Cl− , SO4 2− , Mg2+ , K+ and Ca2+ [1,2,3]. Both natural and anthropogenic components from continental sources may affect NO3 − , SO4 2− , Ca2+ , K+ , and trace metal concentrations over open ocean [1,5,6,7]. Duce et al [5] suggested that reactive nitrogen from anthropogenic sources accounts for a third of the ocean’s external nitrogen supply

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