Thake Henry, Jenkins Stephen J
Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.
Langmuir. 2025 Jul 1;41(25):16315-16327. doi: 10.1021/acs.langmuir.5c01587. Epub 2025 Jun 18.
We present first-principles dynamic simulations of molecular fluorine dissociatively adsorbing on clean C{001} and identify a range of possible outcomes depending upon the interplay of impact site, molecular orientation, and surface temperature. These include adsorption of a single fluorine atom with desorption of the other, in which case both the surface and the isolated atom gain radical character. In most scenarios, however, both fluorine atoms adsorb, either at opposite ends of a single surface dimer or on two such dimers. In the former situation the reaction end-point is closed-shell in nature, whereas in the latter the surface acquires singlet diradical character.
我们展示了分子氟在清洁的C{001}上解离吸附的第一性原理动态模拟，并根据撞击位点、分子取向和表面温度的相互作用确定了一系列可能的结果。这些结果包括一个氟原子吸附而另一个脱附，在这种情况下，表面和孤立的原子都获得自由基特性。然而，在大多数情况下，两个氟原子都会吸附，要么在单个表面二聚体的相对两端，要么在两个这样的二聚体上。在前一种情况下，反应终点本质上是闭壳层的，而在后一种情况下，表面获得单重态双自由基特性。
