Núñez-Pertíñez Samuel, Wilks Thomas R
School of Chemistry, University of Birmingham, Birmingham, United Kingdom.
Front Chem. 2020 Jan 31;8:41. doi: 10.3389/fchem.2020.00041. eCollection 2020.
Translation of genetic information into peptide products is one of the fundamental processes of biology. How this occurred prebiotically, in the absence of enzyme catalysts, is an intriguing question. Nucleic acid-templated synthesis (NATS) promotes reactions by bringing building blocks tethered to complementary DNA strands into close proximity and has been shown to enable peptide synthesis without enzymes-it could therefore serve as a model for prebiotic translation of information stored in nucleic acid sequences into functional peptides. The decomposition of highly reactive DNA adapters has so far limited the effectiveness of NATS, but these studies have been performed exclusively in aqueous solution. Deep eutectic solvents (DESs) have been proposed as a feasible solvent for prebiotic replication of nucleic acids, and here are studied as media for prebiotic translation using NATS as a model. DESs are shown to enhance the stability of DNA-conjugated activated esters, the precursors of peptides. However, this enhanced stability was coupled with decreased amine reactivity that hampered the formation of peptide bonds in DESs. These properties are exploited to demonstrate the storage of DNA-conjugated activated esters in a DES followed by transfer into aqueous buffer to activate the NATS of peptides "on demand." These findings, together with the reported functions of DESs in prebiotic processes, shed light on how DESs could have facilitated the non-enzymatic translation of genetic information into functional peptides on the early Earth.
将遗传信息转化为肽产物是生物学的基本过程之一。在没有酶催化剂的情况下，这一过程在生命起源之前是如何发生的，是一个引人入胜的问题。核酸模板合成（NATS）通过将与互补DNA链相连的构建模块拉近促进反应，并且已被证明能够在没有酶的情况下进行肽合成——因此它可以作为将核酸序列中存储的信息进行生命起源前翻译为功能性肽的模型。到目前为止，高反应性DNA衔接子的分解限制了NATS的有效性，但这些研究都是在水溶液中进行的。深共熔溶剂（DESs）已被提议作为核酸生命起源前复制的可行溶剂，本文以NATS为模型，研究其作为生命起源前翻译的介质。结果表明，DESs可提高肽前体DNA共轭活化酯的稳定性。然而，这种稳定性的提高伴随着胺反应性的降低，这阻碍了DESs中肽键的形成。利用这些特性证明了将DNA共轭活化酯储存在DES中，然后转移到水性缓冲液中以“按需”激活肽的NATS。这些发现，连同DESs在生命起源前过程中已报道的功能，揭示了DESs如何在早期地球上促进遗传信息向功能性肽的非酶促翻译。
