Feng Kun, Solel Ephrath, Schreiner Peter R, Fuchs Harald, Gao Hong-Ying
School of Chemical Engineering and Technology, Tianjin University, 300072 Tianjin, China.
Center for Nanotechnology, Heisenberg Strasse 11, 48149 Münster, Germany.
J Phys Chem Lett. 2021 Apr 8;12(13):3468-3475. doi: 10.1021/acs.jpclett.1c00387. Epub 2021 Apr 1.
We report the on-surface chemistry of diamantanethiols on metal surfaces by combining low-temperature STM studies with quantum mechanical density functional theory computations. First, we examined the spatial configurations of diamantanethiols on metal surfaces, in which the thiol-substrate confinement plays a key role. We then thermally desorbed the diamantanethiols from the substrate surfaces to determine whether the C-S or S-metal bonds preferentially break. Finally, we explored diamantane-4,9-dithiol and its polymerization on metal surfaces, forming linear nanodiamond disulfur chains. This work broadens the fundamental knowledge of functionalized diamondoid behavior on surfaces and provides a novel approach to link diamantane as necklace-chain nanodiamond hybrid materials.
我们通过结合低温扫描隧道显微镜（STM）研究与量子力学密度泛函理论计算，报告了二金刚烷硫醇在金属表面的表面化学。首先，我们研究了二金刚烷硫醇在金属表面的空间构型，其中硫醇 - 底物限制起着关键作用。然后，我们将二金刚烷硫醇从底物表面热解吸，以确定C - S键还是S - 金属键优先断裂。最后，我们探索了金刚烷 - 4,9 - 二硫醇及其在金属表面的聚合，形成线性纳米金刚石二硫链。这项工作拓宽了表面功能化类金刚石行为的基础知识，并提供了一种将金刚烷连接成项链链纳米金刚石杂化材料的新方法。
