莱州湾大气颗粒相中多环芳烃及其衍生物的赋存特征

多环芳烃作为一类典型的持久性有毒物质，一直是环境领域关注的热点和重点，有关多环芳烃衍生物的报道，尤其是有关大气中烷基和硝基多环芳烃的研究报道仍非常缺乏。本研究选取莱州湾刁龙嘴为采集区域，对大气颗粒相样品中16种母体多环芳烃（PAHs）、12种烷基多环芳烃（A–PAHs）和25种硝基多环芳烃（N–PAHs）进行分析。结果表明，16种母体多环芳烃（Σ₁₆PAHs）的浓度范围为517.2 ~ 64124.8 pg/m3；12种烷基化多环芳烃（Σ₁₂A–PAHs）的浓度范围为273.6 ~ 5897.3 pg/m3；25种硝基化多环芳烃（Σ₂₅N–PAHs）的浓度范围为113.5 ~ 1032.3 pg/m3。3种类型多环芳烃的浓度和污染模式均表现出明显的季节变化特征，其中，夏季，2环、3环的PAHs、A–PAHs和N–PAHs比例相对较高，而冬季4环及以上单体的比例偏高。PAHs的特征比值表明，莱州湾刁龙嘴地区PAHs的来源主要以柴油、煤及生物质燃烧为主。Σ₁₆PAHs、Σ₁₂A–PAHs和Σ₂₅N–PAHs与温度均呈现出显著的负相关性（R2 = 0.94，p < 0.01；R2 = 0.61， p < 0.01；R2 = 0.74，p < 0.01），说明温度是影响颗粒相吸附芳烃类物质的一个主要因素。此外，三者之间Pearson相关关系表明，PAHs及其衍生物表现出相同的污染来源和相似的环境行为。

Occurrence of different type polycyclic aromatic hydrocarbon (PAHs) in particle atmosphere of Laizhou Bay

As a type of typical persistent toxic substances, polycyclic aromatic hydrocarbons, have always been the hot spot and key point in the environmental field. However, the reports on derivatives of polycyclic aromatic hydrocarbons, especially the alkyl and nitro polycyclic aromatic hydrocarbons in the atmosphere, are still sparse. In this work, the atmospheric particulate were collected in Diaolongzui site in Laizhou Bay and 16 parent polycyclic aromatic hydrocarbons(PAHs), 12 alkylated polycyclic aromatic hydrocarbons (A-PAHs), and 25 nitrated polycyclic aromatic hydrocarbons (N–PAHs) were determined. The results indicate that the Σ₁₆PAHs concentrations range from 517.2 to 64124.8 pg/m3, the Σ₁₂A–PAHs concentrations range from 273.6 to 5897.3 pg/m3, and the Σ₂₅N–PAHs concentrations range from 113.5 to 1032.3 pg/m3. The concentrations and pollution patterns of the three types of polycyclic aromatic hydrocarbons show obvious seasonal variation characteristics. Among them, the proportion of PAHs, A–PAHs and N–PAHs of ring 2 and 3 is relatively high in summer, while the proportion of monomers with ring 4 and above is relatively high in winter. The characteristic ratios of PAHs indicate that the sources of PAHs in Diaolongzui area are mainly from diesel commission, coal and biomass combustion. The significant negative correlations between Σ₁₆PAHs、Σ₁₂A–PAHs and Σ₂₅N–PAHs (R2 = 0.94, p < 0.01; R2 = 0.61, p < 0.01; R2 = 0.74, p < 0.01) indicate that the temperature is a major factor affecting the adsorption of aromatic hydrocarbons by particulate matter. Furthermore, the Pearson correlation between the three types aromatic hydrocarbons also indicate that PAHs and their derivatives exhibit a same sources and a similar environmental behaviors.