Physikalische Chemie I-Biophysikalische Chemie, Fakultät für Chemie und Chemische Biologie, TU Dortmund, Otto-Hahn-Strasse 4a, Dortmund 44227, Germany.
Lehrstuhl für Theoretische Chemie, Ruhr-Universität Bochum, Bochum 44780, Germany.
Nat Commun. 2017 Mar 30;8:14661. doi: 10.1038/ncomms14661.
The ability of certain RNAs, denoted as ribozymes, to not only store genetic information but also catalyse chemical reactions gave support to the RNA world hypothesis as a putative step in the development of early life on Earth. This, however, might have evolved under extreme environmental conditions, including the deep sea with pressures in the kbar regime. Here we study pressure-induced effects on the self-cleavage of hairpin ribozyme by following structural changes in real-time. Our results suggest that compression of the ribozyme leads to an accelerated transesterification reaction, being the self-cleavage step, although the overall process is retarded in the high-pressure regime. The results reveal that favourable interactions between the reaction site and neighbouring nucleobases are strengthened under pressure, resulting therefore in an accelerated self-cleavage step upon compression. These results suggest that properly engineered ribozymes may also act as piezophilic biocatalysts in addition to their hitherto known properties.
某些 RNA（称为核酶）不仅能够存储遗传信息，还能够催化化学反应，这为 RNA 世界假说提供了支持，该假说被认为是地球早期生命发展的一个可能步骤。然而，这可能是在极端环境条件下进化而来的，包括深海中的 kbar 级压力。在这里，我们通过实时跟踪结构变化来研究压力对发夹核酶自我切割的影响。我们的结果表明，核酶的压缩会导致转酯化反应加速，即自我切割步骤，尽管在高压环境下整个过程会受到阻碍。结果表明，在压力下，反应位点与相邻核碱基之间的有利相互作用得到加强，因此在压缩时自我切割步骤会加速。这些结果表明，经过适当设计的核酶除了具有已知的性质外，还可能作为压敏生物催化剂发挥作用。
