不同地区柴油中正构烷烃碳、氢稳定同位素检验和溯源研究

Examination and Tracing of Stable Isotopes of Carbon and Hydrogen in Diesel Oil from Different Regions

  • 摘要: 在涉火案件中柴油通常被用作助燃剂,探明案件现场柴油的来源是侦破涉火案件的重点工作。柴油正构烷烃中的碳、氢稳定同位素包含了原料来源等地理特征信息,借此可推断柴油产地,为破获涉及柴油的放火案件提供帮助。本研究利用气相色谱-同位素比质谱(GC-IRMS)法对我国4个地区的44种不同柴油中n-C12n-C19正构烷烃组分进行碳、氢稳定同位素检测,并考察了判别分析、多层感知器和径向基函数3种模型对柴油生产地区的溯源分析情况。结果表明,利用判别分析模型分析柴油来源时,依靠碳、氢2种元素数据构建的算法模型交叉整体正确率可达89.9%,高于单一元素构建的模型交叉判别正确率。利用正构烷烃碳、氢同位素比值数据构建的多层感知器模型测试集判别正确率为90.0%,径向基函数测试集判别正确率为90.9%。3种模型在分析不同地区样本来源的正确率有差别,在实际应用中需结合多个模型结果进行横向比较,以达到最佳的溯源效果。本研究通过建立柴油的产地溯源模型,可为柴油产地的分析提供有效支撑。

     

    Abstract: Diesel is often used as an accelerant in arson cases, so identifying its source is crucial to the investigation. Stable isotope analysis is a method for detecting molecular elements at the element level. The carbon and hydrogen isotope information of diesel n-alkanes has geographical characteristics reflecting the source of raw materials. Previous studies have successfully established the relationships between field samples and control samples using cluster analysis and discriminant analysis algorithms. However, with increased accessibility, criminals can cross borders more easily, complicating the investigation process. Traditional analytical methods typically rely on known diesel sources to compare isotopic information between the sample and the control material. However, criminals often purchase diesel from different locations and ship it to crime scenes, thus separating control samples from crime scene evidence and complicating further investigation and evidence collection. Therefore, tracing and origin analysis of diesel oil is a necessary condition to improve the diesel oil tracing system based on isotope information. This method supports the investigation of cross-regional fire crimes. In this study, discriminant analysis and neuwere ral network algorithms were used to analyze the carbon and hydrogen isotope data of n-alkanes in diesel samples from Beijing, Gansu, Heilongjiang, Shandong. The corresponding analysis model was established, and the effectiveness of different statistical methods for diesel engine source inference was discussed. The carbon and hydrogen isotopes of n-C12-n-C19 in 44 diesel oil samples from Beijing, Gansu, Heilongjiang, and Shandong were analyzed by gas chromatography-isotope ratio mass spectrometry (GC-IRMS). The results were evaluated using discriminant analysis, multilayer perceptron (MLP) and radial basis function (RBF). The results showed significant regional differences are in the carbon and hydrogen isotope ratios of diesel n-alkanes. When the discriminant analysis algorithm was used to determine the diesel fuel source, the model based on carbon and hydrogen isotope data has a better classification effect than the model based on a single element. Using carbon and hydrogen isotope data as indexes, the source traceability of diesel oil was evaluated by MLP and RBF neural network models. The results showed that the classification accuracies of MLP and RBF models are 90.0% and 90.9%, respectively. Among the three models, the discriminant function model has the highest overall accuracy. However, when the samples from four regions were distinguished by the two neural network models, the classification accuracy of most regions is better than or close to the discriminant analysis model, and some accuracy is lower than the discriminant analysis model. The horizontal comparison of discriminant analysis results should be combined in application to achieve the best traceability results. This study effectively fills the gap in domestic stable isotope diesel source analysis, providing strong technical support for the investigation of diesel arson in the future.

     

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