Integrative metabolomics reveal the organisation of alkaloid biosynthesis in Daphniphyllum macropodum
Integrative metabolomics reveal the organisation of alkaloid biosynthesis in Daphniphyllum macropodum
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DOI：
10.1101/2022.05.25.493403
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发表时间：
2022-05
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通讯作者：
Kaouthar Eljounaidi;Barbara A Radzikowska;C. Whitehead;Susana Conde;William Davis;A. Dowle;Swen Langer;Tony Larson;W. Unsworth;Daphne Ezer;Benjamin R. Lichman
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作者：
Kaouthar Eljounaidi;Barbara A Radzikowska;C. Whitehead;Susana Conde;William Davis;A. Dowle;Swen Langer;Tony Larson;W. Unsworth;Daphne Ezer;Benjamin R. Lichman
虎皮楠生物碱是一种结构多样的含氮化合物，具有多环立体化学丰富的碳骨架。了解植物如何生物合成这些化合物可能会导致更多的访问，允许探索生物活性;然而，很少有人知道他们的生物合成的起源。在这里，我们整合代谢组学方法来映射生物碱分布在Daphniphyllum macropodum植物和组织。我们生成了一种新的非靶向代谢组学工作流程，以突出组织中生物碱分布的趋势，使用不依赖于模糊峰注释的整体方法。液相色谱-质谱和质谱成像分析独立地揭示了生物碱具有基于其骨骼亚型的空间分布模式。不同的生物碱亚型定位表明，生物合成途径在空间上受到控制，中间体从韧皮部运输到表皮，在表皮中进行额外的衍生化。这项研究为今后的虎皮楠生物碱生物合成工作奠定了基础，并强调了如何整合不同的代谢组学策略可以揭示这些化合物在植物中分布的有价值的见解。
Daphniphyllum alkaloids are structurally diverse nitrogen-containing compounds with polycyclic, stereochemically rich carbon skeletons. Understanding how plants biosynthesise these compounds may lead to greater access to allow exploration of bioactivities; however, very little is known about their biosynthetic origins. Here, we integrated metabolomics approaches to map alkaloid distribution across Daphniphyllum macropodum plants and tissues. We generated a novel untargeted metabolomics workflow to highlight trends in alkaloid distribution across tissues, using a holistic approach that does not rely on ambiguous peak annotations. Both liquid-chromatography-mass spectrometry and mass-spectrometry imaging analyses independently revealed that alkaloids have a pattern of spatial distribution based on their skeletal subtypes. The distinct alkaloid subtype localisation suggests the biosynthetic pathway is controlled spatially with intermediates transported from the phloem to the epidermis where they undergo additional derivatization. This study sets the stage for the future work on Daphniphyllum alkaloid biosynthesis and highlights how integrating different metabolomics strategies can reveal valuable insights on these compounds’ distribution within the plant.