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化合物碳同位素-氘同位素揭示的中挥发性烷烃的来源多样性。

Source Diversity of Intermediate Volatility -Alkanes Revealed by Compound-Specific δC-δD Isotopes.

机构信息

State Key Laboratory of Organic Geochemistry, Chinese Academy of Sciences, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou510640, P. R. China.

Key Laboratory of Agro-ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha410125, P.R. China.

出版信息

Environ Sci Technol. 2022 Oct 18;56(20):14262-14271. doi: 10.1021/acs.est.2c02156. Epub 2022 Oct 7.

Abstract

Intermediate volatility organic compounds (IVOCs) are important precursors of secondary organic aerosols, and their sources remain poorly defined. -alkanes represent a considerable portion of IVOCs in atmosphere, which can be well identified and quantified out of the complex IVOC pool. To investigate the potential source diversity of intermediate volatility -alkanes (IVnAs, C-C), we apportioned the sources of IVnAs in the atmosphere of four North China cities, based on their compound-specific δC-δD isotope compositions and Bayesian model analysis. The concentration level of IVnAs reached 1195 ± 594 ng/m. The δC values of IVnAs ranged -32.3 to -27.6‰ and δD values -161 to -90‰. The δD values showed a general increasing trend toward higher carbon number alkanes, albeit a zigzag odd-even prevalence. Bayesian MixSIAR model using δC and δD compositions revealed that the source patterns of individual IVnAs were inconsistent; the relative contributions of liquid fossil combustion were higher for lighter IVnAs (C-C), while those of coal combustion were higher for heavier IVnAs (C-C). This result agrees with principal component analysis of the dual isotope data. Overall, coal combustion, liquid fossil fuel combustion, and biomass burning contributed about 47.8 ± 0.1, 35.7 ± 4.0, and 16.3 ± 4.2% to the total IVnAs, respectively, highlighting the importance of coal combustion as an IVnA source in North China. Our study demonstrates that the dual-isotope approach is a powerful tool for source apportionment of atmospheric IVOCs.

摘要

中等挥发性有机化合物(IVOCs)是二次有机气溶胶的重要前体,但它们的来源仍未得到明确界定。正构烷烃是大气中 IVOCs 的重要组成部分,可以从复杂的 IVOC 混合物中很好地识别和定量。为了研究中等挥发性正构烷烃(IVnAs,C-C)的潜在源多样性,我们基于其化合物特异性 δC-δD 同位素组成和贝叶斯模型分析,对华北四个城市大气中的 IVnAs 来源进行了分配。IVnAs 的浓度水平达到 1195±594ng/m。IVnAs 的 δC 值范围为-32.3 至-27.6‰,δD 值范围为-161 至-90‰。尽管奇数和偶数烷烃的 δD 值存在波动,但随着碳数的增加,δD 值呈现出总体增加的趋势。使用 δC 和 δD 组成的贝叶斯 MixSIAR 模型表明,单个 IVnAs 的源模式不一致;对于较轻的 IVnAs(C-C),液体化石燃料燃烧的相对贡献较高,而对于较重的 IVnAs(C-C),则是煤炭燃烧的相对贡献较高。这一结果与双同位素数据的主成分分析一致。总体而言,煤炭燃烧、液体化石燃料燃烧和生物质燃烧分别对总 IVnAs 的贡献约为 47.8±0.1%、35.7±4.0%和 16.3±4.2%,突出了煤炭燃烧作为华北地区 IVnA 源的重要性。我们的研究表明,双同位素方法是大气 IVOCs 源分配的有力工具。

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