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中国上海环境空气中的颗粒态汞:粒径分布、气粒分配及与碳质组成的关系。

Particulate mercury in ambient air in Shanghai, China: Size-specific distribution, gas-particle partitioning, and association with carbonaceous composition.

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.

School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei, 230009, China.

出版信息

Environ Pollut. 2018 Jul;238:543-553. doi: 10.1016/j.envpol.2018.03.088. Epub 2018 Mar 30.

Abstract

Mercury (Hg) has a complex atmospheric transformation cycle and acts as a global pollutant. Size-specific particle bound mercury (PBM) was implemented in different functional (industrial, urban and suburban) areas in Shanghai, China. The total concentration of 13-staged PBM (rang of 0.01-18.0 μm) varied of 99.0-611 pg/m, with an average value of 318 ± 144 pg/m. The Gaoqiao petrochemical industry (GQPI) site showed the highest concentrations, whereas the suburban Shanghai Jiao Tong University (SJTU) displayed the lowest. The PBM in nucleation, accumulation and coarse modes were 7.63-96.7, 69.5-455, and 9.43-176 pg/m, respectively, and the fractions of 0.56-1.00 and 0.32-0.56 μm were the two most abundant. Both OC and EC displayed unimodal distribution patterns (peak of 0.56-1.00 μm) at GQPI, while bimodal distributions were observed at urban and suburban sites. Statistically positive correlations between the overall PBM and the corresponding PM and carbonaceous compounds (r = 0.38-0.54, p < 0.01), indicating their similar origins and OC/EC enhanced gaseous mercury forming PBM. The gas-particle partition model predicted gaseous oxidized mercury (GOM) were 253 ± 133, 237 ± 122, and 257 ± 144 pg/m for GQPI, SAES and SJTU, respectively. The particle proportions of divalent mercury in the fraction of 0.32-1.00 μm were substantial (>80%), but smaller (<50%) for nucleation and coarse modes. The fraction of 9.90-18.00 μm occupied nearly 50% of the overall dry deposition fluxes of mercury. These finding highlight the emissions from different mercury and OC/EC origins, caused different size-specific distributions of PBM, which further affect their gas-particle partitioning and dry deposition of mercury species.

摘要

汞(Hg)具有复杂的大气转化循环,是一种全球性污染物。在中国上海的不同功能(工业、城市和郊区)区域实施了基于颗粒大小的汞(PBM)。13 级分段 PBM(0.01-18.0 μm 范围)的总浓度为 99.0-611 pg/m,平均值为 318±144 pg/m。高桥石化工业区(GQPI)的浓度最高,而郊区的上海交通大学(SJTU)的浓度最低。成核、积累和粗模态中的 PBM 分别为 7.63-96.7、69.5-455 和 9.43-176 pg/m,0.56-1.00 和 0.32-0.56 μm 的分数是最丰富的两种。OC 和 EC 在 GQPI 都呈现单峰分布模式(0.56-1.00 μm 峰),而在城市和郊区站点则观察到双峰分布。整体 PBM 与相应的 PM 和含碳化合物之间存在显著的正相关关系(r=0.38-0.54,p<0.01),表明它们具有相似的来源,OC/EC 增强了气态汞形成 PBM。气粒分配模型预测 GQPI、SAES 和 SJTU 的气态氧化汞(GOM)分别为 253±133、237±122 和 257±144 pg/m。0.32-1.00 μm 粒径段二价汞的颗粒比例较大(>80%),但成核和粗模态较小(<50%)。9.90-18.00 μm 粒径段占汞总干沉积通量的近 50%。这些发现强调了不同汞和 OC/EC 来源的排放,导致了 PBM 的不同粒径分布,进一步影响了它们的气粒分配和汞物种的干沉积。

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