Formation of methylglyoxal (CH3C(O)CHO) in interstellar analog ices – a key intermediate in cellular metabolism,Physical Chemistry Chemical Physics

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Formation of methylglyoxal (CH3C(O)CHO) in interstellar analog ices – a key intermediate in cellular metabolism
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2024-08-26 , DOI: 10.1039/d4cp02779e
Jia Wang _{1,

2} , Joshua H Marks _{1,

2} , Evgenia A Batrakova ₃ , Sergey O Tuchin ₃ , Ivan O Antonov ₃ , Ralf I Kaiser _{1,

2}

Affiliation

Ketoaldehydes are key intermediates in biochemical processes including carbohydrate, lipid, and amino acid metabolism. Despite their crucial role in the interstellar synthesis of essential biomolecules necessary for the Origins of Life, their formation mechanisms have largely remained elusive. Here, we report the first bottom-up formation of methylglyoxal (CH₃C(O)CHO)—the simplest ketoaldehyde—through the barrierless recombination of the formyl (HĊO) radical with the acetyl (CH₃ĊO) radical in low-temperature interstellar ice analogs upon exposure to energetic irradiation as proxies of galactic cosmic rays. Utilizing vacuum ultraviolet photoionization reflectron time-of-flight mass spectrometry and isotopic substitution studies, methylglyoxal and its enol tautomer 2-hydroxypropenone (CH₃C(OH)CO) were identified in the gas phase during the temperature-programmed desorption of irradiated carbon monoxide–acetaldehyde (CO–CH₃CHO) ices, suggesting their potential as promising candidates for future astronomical searches. Once synthesized in cold molecular clouds, methylglyoxal can serve as a key precursor to sugars, sugar acids, and amino acids. Furthermore, this work provides the first experimental evidence for tautomerization of a ketoaldehyde in interstellar ice analogs, advancing our fundamental knowledge of how ketoaldehydes and their enol tautomers can be synthesized in deep space.

中文翻译：

星际模拟冰中甲基乙二醛 (CH3C(O)CHO) 的形成——细胞代谢的关键中间体

酮醛是碳水化合物、脂质和氨基酸代谢等生化过程中的关键中间体。尽管它们在生命起源所需的基本生物分子的星际合成中发挥着至关重要的作用，但它们的形成机制在很大程度上仍然难以捉摸。在这里，我们报告了首次自下而上形成甲基乙二醛（CH ₃ C(O)CHO）——最简单的酮醛——通过甲酰基（HĊO）自由基与乙酰基（CH ₃ ĊO）自由基在低温下的无垒重组。暴露于高能辐射下的星际冰类似物作为银河宇宙射线的代表。利用真空紫外光电离反射飞行时间质谱和同位素替代研究，在辐照一氧化碳的程序升温解吸过程中，在气相中鉴定出甲基乙二醛及其烯醇互变异构体 2-羟基丙烯酮 (CH ₃ C(OH)CO) –乙醛（CO-CH ₃ CHO）冰，表明它们有潜力成为未来天文搜索的有希望的候选者。一旦在冷分子云中合成，甲基乙二醛就可以作为糖、糖酸和氨基酸的关键前体。此外，这项工作为星际冰类似物中酮醛互变异构化提供了第一个实验证据，增进了我们对如何在深空合成酮醛及其烯醇互变异构体的基础知识。

更新日期：2024-08-26

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