Desorption Electrospray Ionization Imaging Mass Spectrometry as a Tool for Investigating Model Prebiotic Reactions on Mineral Surfaces
Desorption Electrospray Ionization Imaging Mass Spectrometry as a Tool for Investigating Model Prebiotic Reactions on Mineral Surfaces
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DOI：
10.1021/ac303202n
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发表时间：
2013-02-05
影响因子：
7.4
通讯作者：
Fernandez, Facundo M.
中科院分区：
文献类型：
--
作者：
Bennett, Rachel V.;Cleaves, H. James, II;Fernandez, Facundo M.
甲酰胺的矿物辅助热分解（HCONH2）是一种被大量研究的模型益生元反应，它为导致原始信息聚合物的化学构建块的合理途径提供了有价值的见解。迄今为止，大多数努力都集中在分析溶液中释放的甲酰胺反应产物，尽管有几项研究考察了矿物催化剂在促进这种化学反应中的作用。我们在此表明，通过解吸电喷雾电离-质谱成像（DESI-MSI）对活性矿物表面的直接研究为矿物表面在反应产物形成中的重要作用提供了一个新的视角。作为一个原理证明的例子，我们表明DESI-MSI允许以最少的样品制备对异质花岗岩样品上产生的分子产物进行讯问。通过DESI-MSI成功检测到嘌呤和嘧啶核碱基及其衍生物，产物的空间分布与矿物微环境有较强的相关性。据我们所知，这项研究是DESI-MSI首次应用于研究复杂和多孔矿物表面及其在化学演化中的作用。这种DESI-MSI方法通常适用于涉及矿物的各种反应或其他过程。
Mineral-assisted thermal decomposition of formamide (HCONH2) is a heavily studied model prebiotic reaction that has offered valuable insights into the plausible pathways leading to the chemical building blocks of primordial informational polymers. To date, most efforts have focused on the analysis of formamide reaction products released in solution, although several studies have examined the role of mineral catalysts in promoting this chemistry. We show here that the direct investigation of reactive mineral surfaces by desorption electrospray ionization-mass spectrometry imaging (DESI-MSI) gives a new perspective on the important role of the mineral surface in the formation of reaction products. As a proof-of-principle example, we show that DESI-MSI allows interrogation of the molecular products produced on heterogeneous granite samples with minimal sample preparation. Purine and pyrimidine nucleobases and their derivatives are successfully detected by DESI-MSI, with a strong correlation of the spatial product distribution with the mineral microenvironment. To our knowledge, this study is the first application of DESI-MSI to the study of complex and porous mineral surfaces and their roles in chemical evolution. This DESI-MSI approach is generally applicable to a wide range of reactions or other processes involving minerals.