利用π-π堆叠相互作用设计Cu(II)核苷酸配合物:晶体结构和氨基酸对映体识别

IF 3.4 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Yaqoot Khan, , , Ke Zhao, , , Hafiz Zeshan Aqil, , , Karim Youssef Nabat, , , Hongwei Ma, , and , Hui Li*, 
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引用次数: 0

摘要

手性氨基酸的立体选择性识别仍然是仿生化学的一个基本挑战。在这里,我们报道了铜(II)配位复合物(C-1)的单晶,它作为受体,利用π-π堆叠相互作用作为区分色氨酸(Trp)和组氨酸(His)对映体的主要机制。C-1由单磷酸脱氧胞苷(dCMP)和1,10-菲罗啉配体构成,采用一维结构,通过立体特异性芳香相互作用选择性结合l-和d-对映体。紫外可见滴定显示l-色氨酸的吸光度比d-色氨酸增加了10倍,而圆二色性(CD)光谱显示出明显的棉花效应,直接归因于吲哚/咪唑侧链和C-1芳香骨架之间的π-π堆积。DFT计算表明π-π结合能(- 0.49至- 1.20 eV)是对映体选择性识别的驱动力,几何排列增强了l-和d-对映体的稳定性。通过优先考虑π驱动的相互作用而不是氢键,C-1实现了精确的对映体选择性,可与生物系统相媲美。这项工作建立了π-π堆叠作为合成受体的设计原则,促进了基于非共价分子识别的自适应手性传感。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Design of Cu(II) Nucleotide Coordination Complex by Engineered π-π Stacking Interaction: Crystal Structure and Enantiomer Recognition of Amino Acids

Design of Cu(II) Nucleotide Coordination Complex by Engineered π-π Stacking Interaction: Crystal Structure and Enantiomer Recognition of Amino Acids

The stereoselective recognition of chiral amino acids remains a fundamental challenge in biomimetic chemistry. Here, we report a single crystal of copper(II) coordination complex (C-1), which functions as a receptor, engineered by leveraging π-π stacking interactions as the primary mechanism for discriminating enantiomers of tryptophan (Trp) and histidine (His). Constructed from deoxycytidine monophosphate (dCMP) and 1,10-phenanthroline ligands, C-1 adopts a one-dimensional architecture that selectively binds l- and d-enantiomers through stereospecific aromatic interactions. UV–visible titrations reveal a 10-fold increase in absorbance for l-Trp compared to d-Trp, while circular dichroism (CD) spectra exhibit distinct Cotton effects, directly attributed to π-π stacking between the indole/imidazole side chains and the aromatic framework of C-1. DFT calculations reveal π-π binding energies (−0.49 to −1.20 eV) as the driving force for enantioselective recognition, with geometric alignment enhancing stabilization of both l- and d-enantiomers. By prioritizing π-driven interactions over hydrogen bonding, C-1 achieves precise enantioselectivity, comparable to biological systems. This work establishes π-π stacking as a design principle for synthetic receptors, facilitating adaptive chiral sensing based on noncovalent molecular recognition.

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来源期刊
Crystal Growth & Design
Crystal Growth & Design 化学-材料科学:综合
CiteScore
6.30
自引率
10.50%
发文量
650
审稿时长
1.9 months
期刊介绍: The aim of Crystal Growth & Design is to stimulate crossfertilization of knowledge among scientists and engineers working in the fields of crystal growth, crystal engineering, and the industrial application of crystalline materials. Crystal Growth & Design publishes theoretical and experimental studies of the physical, chemical, and biological phenomena and processes related to the design, growth, and application of crystalline materials. Synergistic approaches originating from different disciplines and technologies and integrating the fields of crystal growth, crystal engineering, intermolecular interactions, and industrial application are encouraged.
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