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Water-Induced Chiral Separation on a Au(111) Surface
ACS Nano ( IF 15.8 ) Pub Date : 2021-10-15 , DOI: 10.1021/acsnano.1c07842 Donglin Li 1 , Luye Sun 2, 3 , Yuanqi Ding 1 , Mengxi Liu 2, 3 , Lei Xie 1 , Yinfu Liu 1 , Lina Shang 1 , Yangfan Wu 2, 4 , Hui-Jun Jiang 5 , Lifeng Chi 6 , Xiaohui Qiu 2, 3 , Wei Xu 1
ACS Nano ( IF 15.8 ) Pub Date : 2021-10-15 , DOI: 10.1021/acsnano.1c07842 Donglin Li 1 , Luye Sun 2, 3 , Yuanqi Ding 1 , Mengxi Liu 2, 3 , Lei Xie 1 , Yinfu Liu 1 , Lina Shang 1 , Yangfan Wu 2, 4 , Hui-Jun Jiang 5 , Lifeng Chi 6 , Xiaohui Qiu 2, 3 , Wei Xu 1
Affiliation
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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 in vivo. Water has been demonstrated in vitro 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–H2O–U)2 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 in vivo.
中文翻译：
Au(111) 表面的水诱导手性分离
面对生命中手性起源的科学问题，水被认为在驱动许多体内生物相关过程中起着至关重要的作用。水已在体外得到证实与手性产生、放大和反转有关，而其潜在机制仍未完全了解。因此，迫切需要单分子水平的真实空间证据来了解水分子在生物分子手性相关问题中的作用。在这里，我们选择了一种 RNA 碱基，即生物分子尿嘧啶 (U)，它自组装成外消旋氢键结构。令人惊讶的是，在暴露于水时，外消旋结构可以转化为同手性涉水结构，从而导致表面出现意想不到的手性分离。手性分离的起源是由于水与 U 分子的特定位点之间的优先结合，导致形成能量最有利的同手性 (U–H 2 O–U) 2簇作为随后手性扩增的种子。这种水驱动的自组装过程也可以扩展到其他生物相关系统，如氨基酸和糖，这将为水分子在体内同手性起源中可能发挥的作用提供一般见解。
更新日期：2021-10-26
中文翻译：
Au(111) 表面的水诱导手性分离
面对生命中手性起源的科学问题，水被认为在驱动许多体内生物相关过程中起着至关重要的作用。水已在体外得到证实与手性产生、放大和反转有关，而其潜在机制仍未完全了解。因此，迫切需要单分子水平的真实空间证据来了解水分子在生物分子手性相关问题中的作用。在这里，我们选择了一种 RNA 碱基，即生物分子尿嘧啶 (U)，它自组装成外消旋氢键结构。令人惊讶的是，在暴露于水时，外消旋结构可以转化为同手性涉水结构，从而导致表面出现意想不到的手性分离。手性分离的起源是由于水与 U 分子的特定位点之间的优先结合，导致形成能量最有利的同手性 (U–H 2 O–U) 2簇作为随后手性扩增的种子。这种水驱动的自组装过程也可以扩展到其他生物相关系统，如氨基酸和糖，这将为水分子在体内同手性起源中可能发挥的作用提供一般见解。
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