Interdisciplinary Materials Research Center, College of Materials Science and Engineering, Tongji University, Shanghai 201804, People's Republic of China.
CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, People's Republic of China.
ACS Nano. 2021 Oct 26;15(10):16896-16903. doi: 10.1021/acsnano.1c07842. Epub 2021 Oct 15.
Facing the scientific question of the origin of chirality in life, water is considered to play a crucial role in driving many biologically relevant processes . Water has been demonstrated to be related to chiral generation, amplification, and inversion, while the underlying mechanism is still not fully understood. Real-space evidence at the single-molecule level is thus urgently required to understand the role of water molecules in biomolecular chirality related issues. Herein, we choose one of the RNA bases, the biomolecule uracil (U), which self-assembles into racemic hydrogen-bonded structures. Upon water exposure, surprisingly, racemic structures could be transformed to homochiral water-involved structures, resulting in an unexpected chiral separation on the surface. The origin of chiral separation is due to preferential binding between water and the specific site of U molecules, which leads to the formation of the energetically most favorable homochiral (U-HO-U) cluster as seed for subsequent chiral amplification. Such a water-driven self-assembly process may also be extended to other biologically relevant systems such as amino acids and sugars, which would provide general insights into the role that water molecules may play in the origin of homochirality
面对生命手性起源的科学问题,水被认为在驱动许多与生物学相关的过程中起着至关重要的作用。水已被证明与手性的产生、放大和反转有关,但其潜在机制仍未完全理解。因此,迫切需要在单分子水平的实空间证据来理解水分子在与生物分子手性相关问题中的作用。在本文中,我们选择了一种 RNA 碱基,即生物分子尿嘧啶(U),它可以自组装成外消旋氢键结构。令人惊讶的是,在水暴露后,外消旋结构可以转化为同手性的水参与结构,导致表面上出现意想不到的手性分离。手性分离的起源是由于水与 U 分子特定部位之间的优先结合,导致形成能量上最有利的同手性(U-HO-U)簇,作为后续手性放大的种子。这种水驱动的自组装过程也可能扩展到其他与生物学相关的系统,如氨基酸和糖,这将为水分子在手性起源中的作用提供更普遍的见解。