Department of Physics, Shaanxi University of Science & Technology, Xi'an, 710021, China.
Department of Physics, Shaanxi University of Science & Technology, Xi'an, 710021, China.
J Mol Graph Model. 2023 Jul;122:108494. doi: 10.1016/j.jmgm.2023.108494. Epub 2023 Apr 18.
The sulfur adsorption on gold surface is a hot topic in catalysis, electrochemistry and chemical sensors. However, the multiple structures of adsorbed sulfur and sulfur-induced reconstruction in gold substrate topography are still open problems until now. Here we performed an extensively study on sulfur adsorption on Au(111) surface based on First-Principles calculation. Our results show that the sulfur adsorption with additional Au atoms is not favorable. Thus, the well-known lifting of the herringbone reconstruction of Au(111) after sulfur adsorption can't be attributed to the lifting gold atoms. More importantly, we proposed an extremely stable configuration of S-Au(111) surface characterized by (√3 × √3)R30° at 0.33 coverage, in which each S atom is chemisorbed in 3-fold coordinated sites and all the surface-Au atoms are terminated. Finally, the good agreement between our simulated STM and LEED images and experimental observations illuminates the truth that our proposed configuration is also favorable in experiment. This super stable S-adsorbed surface can be used as a starting point for the growth of two dimensional transition metal sulfides.
硫在金表面的吸附是催化、电化学和化学传感器领域的一个热门话题。然而，直到现在，吸附态硫的多种结构以及硫诱导的金衬底形貌重构仍然是悬而未决的问题。在这里，我们基于第一性原理计算对 Au(111)表面上的硫吸附进行了广泛的研究。我们的结果表明，硫与额外的金原子的吸附是不利的。因此，众所周知的硫吸附后金(111)的非晶重构不能归因于提升的金原子。更重要的是，我们提出了一种非常稳定的 S-Au(111)表面结构，在 0.33 的覆盖率下，其特征为 (√3×√3)R30°，其中每个 S 原子都以三配位的方式化学吸附，所有的表面 Au 原子都被终止。最后，我们模拟的 STM 和 LEED 图像与实验观察之间的良好一致性表明，我们提出的结构在实验中也是有利的。这种超稳定的硫吸附表面可以作为二维过渡金属硫化物生长的起点。
