Compound class specific 14C analysis of polycyclic aromatic hydrocarbons associated with PM10 and PM1.1 aerosols from residential areas of suburban Tokyo.
Compound class specific 14C analysis of polycyclic aromatic hydrocarbons associated with PM10 and PM1.1 aerosols from residential areas of suburban Tokyo.
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DOI：
10.1021/es052407f
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发表时间：
2006-06
影响因子：
11.4
通讯作者：
H. Kumata;M. Uchida;Eisuke Sakuma;T. Uchida;K. Fujiwara;M. Tsuzuki;M. Yoneda;Y. Shibata
中科院分区：
文献类型：
--
作者：
H. Kumata;M. Uchida;Eisuke Sakuma;T. Uchida;K. Fujiwara;M. Tsuzuki;M. Yoneda;Y. Shibata
采用化合物类别特异性放射性碳分析（CCSRA）对日本东京郊区一个居民区大气颗粒物（PM 10和PM 1.1）中的多环芳烃（PAHs）进行了分析，并研究了其季节和粒径的变化。来源诊断异构体对比率表明，混合的贡献，从石油燃烧和生物质和煤燃烧的多环芳烃在APM。APM中δ 14 C-PAHs的含量范围为-787 ~-514 ‰，表明化石燃料燃烧的影响占主导地位。PM10和PM1.1中5-6环（HMW）多环芳烃的δ 14 C值均高于3-4环（LMW）多环芳烃。HMW-PAHs的δ 14 C值表明，夏季生物质燃烧贡献大于冬季，且没有明显的粒径变化。相反，δ 14 C的低分子量物质表现出更大的贡献，从化石来源在夏季和较大的颗粒（PM10）。这一发现可以初步归因于化石多环芳烃从石油源蒸发的再冷凝。14 C同位素质量平衡方法估计，生物质燃烧贡献了17-45%的多环芳烃负担在东京郊区，和生物质多环芳烃的增加约占冬季的LMW-和HMW-PAH的海拔的27%和22%，分别。这些都远远超出了预期的CO2和燃烧材料在日本的排放统计，并强调生物质燃烧作为多环芳烃的来源的重要性，这反过来又证明了实用程序和现场为基础的源评估的意义，通过使用CCSRA的有效监管大气污染的多环芳烃。
Compound class specific radiocarbon analysis (CCSRA) was performed for polycyclic aromatic hydrocarbons (PAHs) associated with airborne particulate matter (APM) with diameter <10 microm (PM10) and <1.1 microm (PM1.1) collected from a residential area of suburban Tokyo, Japan, and seasonal and particle-size radiocarbon variations were investigated. Source diagnostic isomer pair ratios indicated mixed contributions from petroleum combustion and from biomass and coal combustion to the PAHs in APM. The delta14C- PAHs in APM, ranging from -787 to -514 per thousand, indicated dominance of fossil fuel combustion. The delta14C of 5-6 rings (HMW) PAHs were higher than the 3-4 rings (LMW) species in both PM10 and PM1.1 samples. The delta14C of HMW-PAHs indicated greater biomass-burning contributions in summer than in winter and no apparent particle-size variation. Conversely, the delta14C of LMW species showed a greater contribution from fossil sources in summer and in larger particles (PM10). This finding could be tentatively attributed to the recondensation of fossil-PAHs vaporized from petroleum sources. A 14C isotopic mass balance approach estimated that biomass burning contributes 17-45% of the PAH burden in suburban Tokyo, and that the increase in the biomass-PAH accounts for approximately 27% and 22% of winter-time elevation of LMW- and HMW-PAHs, respectively. These are far exceeding what is expected from the emission statistics for CO2 and combusted materials in Japan and emphasizing the importance of biomass-burning as a source of PAHs; which, in turn, demonstrates the utility and the significance of field-based source assessment by using CCSRA for an effective regulation of atmospheric pollution by PAHs.