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大气萘的三重同位素(δC、δH 和 ΔC)组成及其来源解析:一种关键的中等挥发性有机化合物(IVOCs)示踪物。

Triple Isotopes (δC, δH, and ΔC) Compositions and Source Apportionment of Atmospheric Naphthalene: A Key Surrogate of Intermediate-Volatility Organic Compounds (IVOCs).

机构信息

State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, People's Republic of China.

University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China.

出版信息

Environ Sci Technol. 2020 May 5;54(9):5409-5418. doi: 10.1021/acs.est.0c00075. Epub 2020 Apr 16.

Abstract

Naphthalene (NAP), as a surrogate of intermediate-volatility organic compounds (IVOCs), has been proposed to be an important precursor of secondary organic aerosol (SOA). However, the relative contribution of its emission sources is still not explicit. This study firstly conducted the source apportionment of atmospheric NAP using a triple-isotope (δC, δH, and ΔC) technique combined with a Bayesian model in the Beijing-Tianjin-Hebei (BTH) region of China. At the urban sites, stable carbon (-27.7 ± 0.7‰, δC) and radiocarbon (-944.0 ± 20.4‰, ΔC) isotope compositions of NAP did not exhibit significant seasonal variation, but the deuterium system showed a relatively more H depleted signature in winter (-86.7 ± 8.9‰, δH) in comparison to that in summer (-56.4 ± 3.9‰, δH). Radiocarbon signatures indicated that 95.1 ± 1.8% of NAP was emitted from fossil sources in these cities. The Bayesian model results indicated that the emission source compositions in the BTH urban sites had a similar pattern. The contribution of liquid fossil combustion was highest (46.7 ± 2.6%), followed by coal high-temperature combustion (26.8 ± 7.1%), coal low-temperature combustion (18.9 ± 6.4%), and biomass burning (7.6 ± 3.1%). At the suburban site, the contribution of coal low-temperature combustion could reach 70.1 ± 6.4%. The triple-isotope based approach provides a top-down constraint on the sources of atmospheric NAP and could be further applied to other IVOCs in the ambient atmosphere.

摘要

萘(NAP)作为挥发性有机化合物(IVOCs)的替代物,已被提出是二次有机气溶胶(SOA)的重要前体。然而,其排放源的相对贡献仍不明确。本研究首次在中国京津冀地区采用三重同位素(δC、δH 和 ΔC)技术与贝叶斯模型相结合,对大气 NAP 的来源进行了分配。在城市站点,NAP 的稳定碳(-27.7 ± 0.7‰,δC)和放射性碳(-944.0 ± 20.4‰,ΔC)同位素组成没有明显的季节性变化,但氘系统在冬季(-86.7 ± 8.9‰,δH)表现出相对更贫氘的特征,而在夏季(-56.4 ± 3.9‰,δH)则表现出更贫氘的特征。放射性碳特征表明,这些城市中 95.1 ± 1.8%的 NAP 是由化石源排放的。贝叶斯模型结果表明,京津冀城市站点的排放源组成具有相似的模式。液体化石燃烧的贡献最高(46.7 ± 2.6%),其次是高温煤燃烧(26.8 ± 7.1%)、低温煤燃烧(18.9 ± 6.4%)和生物质燃烧(7.6 ± 3.1%)。在郊区站点,低温煤燃烧的贡献可达到 70.1 ± 6.4%。基于三重同位素的方法为大气 NAP 的来源提供了自上而下的约束,并且可以进一步应用于环境空气中的其他 IVOCs。

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