Ruiqi Li, Quanzheng Deng, Lu Han, Tianwei Ouyang, Shunai Che, Yuxi Fang
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引用次数: 0
摘要
D-氨基酸在少数生物中过量存在,对海洋无脊椎动物至关重要,与大多数生物中更常见的L-氨基酸形成鲜明对比。自然系统中 D-氨基酸对映体过量的局部前生物起源仍然是一个未解之谜。在这里,我们展示了通过在天然黄铁矿上对α-酮酸进行光催化还原胺化而形成对映体过量(ee)的D-氨基酸。生成的各种氨基酸的 ee 值范围为 14.5-42.4%。据推测,黄铁矿表面原子的波浪形排列导致了 D-氨基酸的优先形成。这项研究揭示了黄铁矿固有的不对称光催化活性,从而拓展了人们对不对称催化机理和无机晶体手性的理解。此外,它还为 D-氨基酸的前生物形成提供了一条可信的途径,为自然系统中 D-氨基酸对映体过量的起源提供了进一步的证据。
Prebiotic formation of enantiomeric excess D-amino acids on natural pyrite
D-amino acids, found in excess in a minority of organisms and crucial for marine invertebrates, contrast with the more common L-amino acids in most life forms. The local prebiotic origin of D-amino acid enantiomeric excess in natural systems remains an unsolved conundrum. Herein, we demonstrate the formation of enantiomeric excess (ee) D-amino acids through photocatalytic reductive amination of α-keto acids on natural pyrite. Various amino acids with ee values in the range of 14.5–42.4%, are formed. The wavy arrangement of atoms on the surface of pyrite is speculated to lead to the preferential formation of D-amino acids. This work reveals the intrinsic asymmetric photocatalytic activity of pyrite, which could expand understandings on mechanism of asymmetric catalysis and chirality of inorganic crystals. Furthermore, it provides a plausible pathway for the prebiotic formation of D-amino acids, adding further evidence to the origin of D-amino acids enantiomeric excess in natural systems.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.