Institute of Environmental Engineering, National Sun Yet-sen University, Taiwan, Republic of China.
School of Geographic Science, Fujian Normal University, Fujian, China.
Environ Sci Pollut Res Int. 2018 Nov;25(32):32332-32345. doi: 10.1007/s11356-018-3093-9. Epub 2018 Sep 18.
This study aims to investigate the spatiotemporal variation, chemical composition, and source apportionment of marine fine particles (PM) as well as their regional transport toward the Matsu Islands located near the coastline of northwestern Taiwan Strait. Four offshore island sites located at the Matsu Islands were selected to conduct both regular and intensive sampling of marine PM. Water-soluble ionic species, metallic elements, and carbonaceous contents were then analyzed to characterize the chemical characteristics of marine PM. In order to identify the potential sources and their contributions to marine PM, chemical mass balance (CMB) receptor model was employed along with the backward trajectory simulation to resolve the source apportionment of marine PM and to explore their transport routes in different seasons. The results showed that high PM concentrations were commonly observed during the northeastern monsoon periods. Additionally, marine PM concentration decreased from the west to the east with the highest PM at the Nankang Island and the lowest PM at the Donyin Island in all seasons, indicating an obvious concentration gradient of PM transported from the continental areas to the offshore islands. In terms of chemical characteristics of PM, the most abundant water-soluble ions of PM were secondary inorganic aerosols (SO, NO, and NH) which accounted for 55-81% of water-soluble ions and 29-52% of marine PM. The neutralization ratios of PM were always less than unity, indicating that NH cannot solely neutralize nss-SO and NO in marine PM at the Matsu Islands. Although crustal elements (Al, Ca, Fe, K, and Mg) dominated the metallic content of marine PM, trace anthropogenic metals (Cd, As, Ni, and Cr) increased significantly during the northeastern monsoon periods, particularly in winter. Organic carbons (OCs) were always higher than elemental carbons (ECs), and the mass ratios of OC and EC were generally higher than 2.2 in all seasons, implying that PM was likely to be aged particles. During the poor air quality periods, major air mass transport routes were the northern transport and the anti-cyclonic circulation routes. Source apportionment results indicated that fugitive soil dusts and secondary aerosols were the major sources of marine PM at the Matsu Islands, while, in winter, biomass burning contributed up to 15% of marine PM. This study revealed that cross-boundary transport accounted for 66~84% of PM at the Matsu Islands, suggesting that marine PM at the Matsu Islands has been highly influenced by anthropogenic emissions from neighboring Fuzhou City as well as long-range transport from Northeast Asia.
本研究旨在调查海洋细颗粒物(PM)的时空变化、化学组成和来源分配,以及它们向位于台湾海峡西北海岸附近的马祖群岛的区域传输。选择马祖群岛的四个近海岛屿站点进行定期和强化的海洋 PM 采样。然后分析水溶性离子物种、金属元素和含碳物质,以表征海洋 PM 的化学特征。为了识别潜在来源及其对海洋 PM 的贡献,采用化学质量平衡(CMB)受体模型结合后向轨迹模拟来解决海洋 PM 的源分配问题,并探讨不同季节的传输路径。结果表明,东北季风期间通常会出现高 PM 浓度。此外,海洋 PM 浓度从西向东递减,在所有季节中,南港岛的 PM 浓度最高,东引岛的 PM 浓度最低,表明 PM 从大陆地区向近海岛屿的传输存在明显的浓度梯度。就 PM 的化学特征而言,PM 中最丰富的水溶性离子是二次无机气溶胶(SO、NO 和 NH),占水溶性离子的 55-81%,占海洋 PM 的 29-52%。PM 的中和比始终小于 1,表明在马祖群岛,NH 不能单独中和海洋 PM 中的 nss-SO 和 NO。尽管地壳元素(Al、Ca、Fe、K 和 Mg)主导了海洋 PM 的金属含量,但痕量人为金属(Cd、As、Ni 和 Cr)在东北季风期间显著增加,尤其是在冬季。有机碳(OCs)总是高于元素碳(ECs),OC 和 EC 的质量比通常在所有季节都高于 2.2,这意味着 PM 可能是老化颗粒。在空气质量较差的时期,主要大气传输路径是北部传输和反气旋环流路径。源分配结果表明,飞散性土壤尘埃和二次气溶胶是马祖群岛海洋 PM 的主要来源,而在冬季,生物质燃烧贡献了高达 15%的海洋 PM。本研究表明,跨界传输占马祖群岛 PM 的 66~84%,表明马祖群岛的海洋 PM 受到来自邻近福州市的人为排放以及来自东北亚的远距离传输的高度影响。