Exploring the complementarity of fast multipulse and multidimensional NMR methods for metabolomics : a chemical ecology case study

This study investigates the potential and complementarity of high-throughput multipulse and multidimensional NMR methods for metabolomics. Three methods are investigated in a chemical ecology case study. They offer a continuum of methods with complementary features in terms of resolution, sensitivity and experiment time. Ultrafast 2D COSY, adiabatic INEPT and SYMAPS HSQC are shown to provide a very good classification ability, comparable to the reference 1D 1H NMR method. Moreover, a detailed analysis of discriminant buckets by supervised statistical analysis shows that all methods are highly complementary, since they are able to highlight discriminant signals that could not be detected by 1D 1H NMR. In particular, fast 2D methods appear very efficient in discriminating signals located in highly crowded regions of the 1H spectrum. Overall, the combination of these recent methods within a single NMR metabolomics workflow allowed maximization of the accessible metabolic information, and also raises exciting possibilities for challenges posed by NMR data analysis in chemical ecology.

本研究探讨了高通量多脉冲多维核磁共振（Nuclear Magnetic Resonance, NMR）方法在代谢组学（metabolomics）中的应用潜力与互补性，并针对一项化学生态学（chemical ecology）案例研究考察了三种方法。这三种方法构成了一套完整的方法谱系，在分辨率、灵敏度与实验时长方面各具互补优势。研究表明，超快速二维相关谱（Ultrafast 2D COSY）、绝热型不灵敏核极化转移增强（adiabatic INEPT）以及SYMAPS型异核单量子相干谱（SYMAPS HSQC）均具备出色的分类能力，可与基准一维氢谱核磁共振（1D ¹H NMR）方法相媲美。此外，通过监督统计分析对判别分箱（discriminant buckets）进行的详细分析显示，所有方法均具有高度互补性：它们能够识别出一维氢谱核磁共振无法检测到的判别信号。尤为值得注意的是，快速二维方法在区分位于氢谱高度拥挤区域的信号方面展现出极高的效率。总体而言，将这些新型方法整合至单一核磁共振代谢组学工作流程中，不仅能够最大化可获取的代谢信息，还为化学生态学领域核磁共振数据分析所面临的诸多挑战带来了极具前景的探索方向。