方形硫族元素键相互作用及其在银表面吸附行为的第一性原理研究

First-principles study of square chalcogen bond interactions and its adsorption behavior on silver surface.

作者信息

Wang Hui, Li Bin, Wang Xiaoting, Yin Fu, Wei Qiaoyu, Wang Xudong, Ni Yuxiang, Wang Hongyan

机构信息

School of Physical Science and Technology, Southwest Jiaotong University, Chengdu 611756, P. R. China.

School of Astronomy and Space Science, University of Science and Technology of China, Hefei 230026, P. R. China.

出版信息

Phys Chem Chem Phys. 2023 Apr 12;25(15):10836-10844. doi: 10.1039/d2cp05825a.

DOI:10.1039/d2cp05825a

PMID:37013689

Abstract

Research on 2Ch⋯2N (Ch = S, Se, Te) square chalcogen interaction has attracted extensive attention in recent years. By search of the Crystal Structure Database (CSD), square chalcogen structures with 2Ch⋯2N interactions were widely found. Herein, dimers of 2,1,3-benzothiadiazole (CNHS), 2,1,3-benzoselenadiazole (CNHSe) and 2,1,3-benzotelluradiazole (CNHTe) from CSD were chosen to construct a square chalcogen bond model. The square chalcogen bond and their adsorption behavior on Ag(110) surfaces have been systematically studied using first principles. Furthermore, partially fluoro-substituted CNHFCh (Ch = S, Se, Te) complexes were also considered for comparison. The results show that in the CNHCh (Ch = S, Se, Te) dimer, the strength of the 2Ch⋯2N square chalcogen bond is in the order of S < Se < Te. In addition, the strength of the 2Ch⋯2N square chalcogen bond is also enhanced by F atom replacement in partially fluoro-substituted CNHFCh (Ch = S, Se, Te) complexes. The self-assembly behavior of dimer complexes on silver surfaces is guided by van der Waals interactions. This work provides theoretical guidance for the application of 2Ch⋯2N square chalcogen bonds in supramolecular construction and materials science.

摘要

近年来，关于2Ch⋯2N（Ch = S、Se、Te）方形硫族元素相互作用的研究受到了广泛关注。通过搜索晶体结构数据库（CSD），广泛发现了具有2Ch⋯2N相互作用的方形硫族元素结构。在此，从CSD中选取2,1,3 - 苯并噻二唑（CNHS）、2,1,3 - 苯并硒二唑（CNHSe）和2,1,3 - 苯并碲二唑（CNHTe）的二聚体来构建方形硫族元素键模型。利用第一性原理系统地研究了方形硫族元素键及其在Ag(110)表面的吸附行为。此外，还考虑了部分氟取代的CNHFCh（Ch = S、Se、Te）配合物进行比较。结果表明，在CNHCh（Ch = S、Se、Te）二聚体中，2Ch⋯2N方形硫族元素键的强度顺序为S < Se < Te。此外，在部分氟取代的CNHFCh（Ch = S、Se、Te）配合物中，F原子取代也增强了2Ch⋯2N方形硫族元素键的强度。二聚体配合物在银表面的自组装行为受范德华相互作用的引导。这项工作为2Ch⋯2N方形硫族元素键在超分子构建和材料科学中的应用提供了理论指导。