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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Water-Mediated Peptide Bond Formation in the Gas Phase: A Model Prebiotic Reaction
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Water-Mediated Peptide Bond Formation in the Gas Phase: A Model Prebiotic Reaction

机译：气相中的水介导的肽键形成：模型益生元反应

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摘要

The emergence of life on the prebiotic Earth must have involved the formation of polypeptides, yet the polymerization of amino acids is thermodynamically unfavorable under biologically relevant aqueous conditions because amino acids are zwitterions in solution and because of the production of a water molecule through a condensation reaction. Many mechanisms for overcoming this thermodynamic unfavorability have been proposed, but the role of gas phase water clusters has not been investigated. We present the thermodynamics of the water-mediated gas phase dimerization reaction of glycine as a model for the atmospheric polymerization of amino acids prior to the emergence of biological machinery. We hypothesize that atmospheric aerosols may have played a major role in the prebiotic formation of peptide bonds by providing the thermodynamic driving force to facilitate increasingly stable linear oligopeptides. In addition, we hypothesize that small aerosols orient amino acids on their surfaces, thus providing the correct molecular orientations to funnel the reaction pathways of peptides through transition states that lead eventually to polypeptide products. Using density functional theory and a thorough configurational sampling technique, we show that the thermodynamic spontaneity of the linear dimerization of glycine in the gas phase can be driven by the addition of individual water molecules.
机译：益生元地球的生命的出现必须涉及多肽的形成，但在生物相关的水性条件下，氨基酸的聚合在生物学相关的水性条件下，因为氨基酸是溶液中的两性化，并且由于通过缩合反应生产水分子。已经提出了许多克服这种热力学不利地的机制，但尚未研究气相水簇的作用。我们介绍了甘氨酸水介导的气相二聚化反应的热力学，作为生物机械出现前氨基酸大气聚合的模型。我们假设通过提供热力学驱动力以促进越来越稳定的线性寡肽，大气气溶胶可能在肽键的益生元形成中发挥了重要作用。此外，我们假设小气溶胶在其表面上定向氨基酸，从而提供通过最终导致多肽产物的过渡状态汇集肽的反应途径的正确分子取向。使用密度函数理论和彻底的配置采样技术，我们表明，通过添加单独的水分子，可以驱动气相中甘氨酸线性二聚体的热力学自发性。

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