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首页> 外文期刊>Journal of chromatography, A: Including electrophoresis and other separation methods >Use of carbon isotopic ratios in nontargeted analysis to screen for anthropogenic compounds in complex environmental matrices
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Use of carbon isotopic ratios in nontargeted analysis to screen for anthropogenic compounds in complex environmental matrices

机译：使用碳同位素比例在非靶向分析中对复杂环境基质中的人为化合物筛选

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Analytical data for ultra-high-performance liquid chromatography (UHPLC), nontargeted, high-resolution, mass-spectrometry (HR/MS) molecular features from a wide array of samples are used to calculate (C1C(n-1))-C-13-C-12/ C-12(n) isotopologue ratios. These ratios increase with molecular carbon number roughly following a trend defined by atmospheric carbon. When the effective source reservoir C-13/C-12 ratio is calculated from the isotopologue ratio (assuming a fractionation factor of unity), features in biotic samples uniformly are tightly grouped, proximate to atmospheric C-13/C-12 ratio. In contrast, features in soil natural organic matter (NOM), dust NOM and anthropogenic compounds range from proximate to relatively divergent from atmospheric C-13/C-12. For the NOM, C-13/C-12 ratios are consistent with an expected preferential volatilization of 12 C, rendering features in soil NOM C-13-enriched and some features in dust NOM C-13-depleted. Anthropogenic compounds tend to diverge most dramatically from atmospheric C-13/C-12, generally toward C-13-depletion, but pesticides we tested tended toward C-13- enriched. This pattern is robust and evident in: i) anthropogenic vs natural features in dust; ii) perfluorinated compounds in standards and as soil contaminants; and iii) sunscreen compounds in commercial products and wastewater. Considering the observed wide C-13/C-12 range for anthropogenic compounds, we suggest Rayleigh distillation during synthetic processes commonly favors one isotope over the other, rendering a source reservoir that is progressively depleted as synthesis proceeds and, consequently, generates a wide variation in C-13/C-12 for man-made products. However, kinetic-isotopic effects and/or synthesis from petroleum/natural gas might contribute to the anthropogenic isotopic signature as well. Regardless of cause,C-13/C-12 can be used to cull HR/MS molecular features that are more likely to be of anthropogenic or non-biotic origin. Published by Elsevier B.V.
机译：用于超高效液相色谱（UHPLC）的分析数据，来自各种样品的分子，高分辨率，质谱（HR / MS）分子特征用于计算（C1C（N-1）） - C. -13-C-12 / C-12（n）同位素比率。这些比率随着大气碳定义的趋势大致增加了分子碳数。当有效源储层C-13 / C-12比从同位素比（假设单位的分馏因子）计算时，生物样品中的特征均匀地分组，靠近大气C-13 / C-12比。相反，土壤天然有机物质（NOM）的特征，灰尘NOM和人为化合物的范围从大气C-13 / C-12的相对发散的范围。对于NOM，C-13 / C-12比率与预期的优先挥发为12℃，土壤中富含土壤C-13富含的一些特征，以及灰尘NOM C-13耗尽的一些特征。通常从大气C-13 / C-12大幅度地偏离的人为化合物，通常朝向C-13耗尽，但我们测试的农药倾向于C-13-富集。这种模式在：i）灰尘中的人为vs天然特征是鲁棒性和明显的; ii）标准的全氟化合物和土壤污染物;和III）商业产品和废水中的防晒化合物。考虑到所观察到的宽的C-13 / C-12范围用于人为化合物，我们建议在合成过程中瑞利蒸馏通常有利于另一个同位素，呈现出逐渐耗尽的源储层，随着合成所得的，因此产生了广泛的变化在C-13 / C-12用于人造产品。然而，石油/天然气的动力学 - 同位素效应和/或合成也可能有助于人为同位素签名。无论原因如何，C-13 / C-12都可用于剔除HR / MS分子特征，其更可能具有人为或非生物起源。由elsevier b.v出版。

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