In current living matter, biopolymers follow specific sequences that give them special properties, such as the sequence of amino acids (AAs) in proteins and peptides. A major challenge for the elucidation of the origins of life lies in understanding how, for example, nonrandom polypeptides have been selected among all the possible ones. While many investigations established plausible prebiotic polymerization pathways, surprisingly, only a few attempted to study the selectivity of these processes. We studied a mineral surface polymerization scenario based on moderate thermal activation of leucine + glutamic acid mixtures on silica. Oligopeptides up to octamers were quantitatively formed in a “clean” prebiotic reaction and analyzed by high-resolution mass spectrometry and Fourier transform ion cyclotron resonance spectrometry for unambiguous molecular assignments. Nontrivial oligomerization selectivities are evidenced in both stoichiometric compositions and AA sequences, while comparable selectivities are not observed in other polymerization scenarios. This must therefore be due to specific catalytic reaction pathways occurring on the SiO₂ surface. A statistical measure of information contained in oligopeptide distributions is proposed. It could be used to follow the evolution of potentially meaningful complexity in biopolymers from the mineral to the biochemical world.

中文翻译：

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生命和分子信息的起源：矿物表面诱导的益生元氨基酸聚合的选择性

在当前的生物中，生物聚合物遵循特定的序列，赋予它们特殊的性质，例如蛋白质和肽中的氨基酸（AAs）序列。阐明生命起源的主要挑战在于了解如何在所有可能的多肽中选择非随机多肽。尽管许多研究建立了合理的益生元聚合途径，但令人惊讶的是，只有少数尝试研究这些过程的选择性。我们研究了基于在二氧化硅上的亮氨酸+谷氨酸混合物适度热活化的矿物表面聚合方案。在“纯净的”益生元反应中定量形成高达八聚体的寡肽，并通过高分辨率质谱和傅里叶变换离子回旋共振光谱法进行分析，以明确分子分配。在化学计量组成和AA序列中都证明了非平凡的低聚选择性，而在其他聚合方案中未观察到可比的选择性。因此，这必须归因于SiO上发生的特定催化反应路径₂面。提出了寡肽分布中所含信息的统计量度。它可以用来追踪生物聚合物从矿物到生化领域潜在有意义的复杂性的演变。