CCS Chemistry最新文献_第3页

Radical-Mediated N–C Crosslinking in the Biosynthesis of Dynobactin A, a Ribosomally-Derived Peptide Targeting Gram-Negative Bacteria 在针对革兰氏阴性菌的核糖体衍生肽 Dynobactin A 的生物合成过程中由自由基介导的 N-C 交联反应

IF 11.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

CCS Chemistry

Pub Date : 2024-10-25 DOI: 10.31635/ccschem.024.202404983

CCS Chemistry, Ahead of Print.

引用次数: 0

Chalcogenoviologen Enhanced Host–Guest Recognition Chalcogenoviologen 增强宿主-宿主识别能力

IF 11.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

CCS Chemistry

Pub Date : 2024-10-25 DOI: 10.31635/ccschem.024.202404812

Yuanning Feng, Xingang Zhao, Daniel A. Appleton, Han Han, Ryan M. Young, Wenqi Liu, Christopher K. Lee, Weixingyue Li, Bai-Tong Liu, Yong Wu, Chun Tang, Aspen X.-Y. Chen, Charlotte L. Stern, Dong Jun Kim, Michael R. Wasielewski, Yunyan Qiu, J. Fraser Stoddart

In the field of supramolecular chemistry, cyclophanes with novel properties are highly sought after since they can be tailored to fulfill specific tasks. In this article, we incorporate chalcogenoviologen-based units into tetracationic cyclophanes, resulting in enhanced host–guest recognition. The cyclophanes can be tuned through the addition of chalcogen bridging atoms—S, Se, and Te—which enhance their rigidity, regulate bond rotation and introduce additional steric bulk. Three cyclophanes containing chalcogen bridging atoms were synthesized and characterized in both the solution and solid states. The energy barriers for their interconversion between syn- and anti-conformations in solution were found to be correlated with chalcogen atom size. The photophysical properties of the cyclophanes are strongly dependent on the chalcogen atomic number, with intersystem crossing rates increasing from S to Se to Te. UV–vis-NIR spectroscopic and fluorometric titrations revealed that the chalcogenoviologen-based cyclophanes exhibit significantly stronger binding with electron-rich guests compared to the well-known, unsubstituted cyclobis(paraquat-p-phenylene). This enhancement in binding can be attributed to restricted rotation within the chalcogenoviologen units. This research provides insight into the rational design and tailored synthesis of cationic cyclophanes.

在超分子化学领域，具有新颖特性的环烷备受追捧，因为它们可以量身定制以完成特定任务。在本文中，我们在四阳离子环烷中加入了基于缩醛的单位，从而增强了主客体的识别能力。通过添加缩醛桥原子-S、Se 和 Te，可以对环烷进行调整，从而增强其刚性、调节键的旋转并引入额外的立体体积。我们合成了三种含有缩醛桥原子的环烷，并在溶液和固体状态下对其进行了表征。研究发现，它们在溶液中的同构型和反构型之间相互转换的能量障碍与查尔根原子的大小有关。环烷的光物理特性与查尔根原子序数密切相关，从 S 到 Se 再到 Te，系统间的交叉率不断增加。紫外-可见-近红外光谱仪和荧光滴定法显示，与众所周知的未取代环双（百草枯-对苯二甲酸）相比，基于链烯的环烷与富电子客体的结合力明显更强。这种结合力的增强可归因于链烯单元内旋转受限。这项研究为阳离子环烷的合理设计和定制合成提供了启示。

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引用次数: 0

Introducing Polymer-to-Polymer Transformation into Multipath Closed-Loop Chemical Recycling by the Ring-Opening Polymerization of Thionolactone for Enhanced Versatility 通过硫代内酯的开环聚合将聚合物到聚合物的转化引入多途径闭环化学循环以提高多功能性

IF 11.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

CCS Chemistry

Pub Date : 2024-10-25 DOI: 10.31635/ccschem.024.202404866

CCS Chemistry, Ahead of Print.