Bohamud T, Reutzel M, Dürr M, Höfer U
Fachbereich Physik und Zentrum für Materialwissenschaften, Philipps-Universität Marburg, D-35032 Marburg, Germany.
J Chem Phys. 2019 Jun 14;150(22):224703. doi: 10.1063/1.5092804.
The reaction dynamics of methanol and water on Si(001) were investigated by means of molecular beam techniques. The initial sticking probability s was determined as a function of the kinetic energy of the incoming molecules, E, and surface temperature, T. For both, methanol and water, a nonactivated reactional channel was observed; the dynamics were found to be determined by the reaction into the datively bonded intermediate state. A low conversion barrier was deduced for the conversion from this intermediate into the final state. It is attributed to the reaction mechanism, which proceeds via proton transfer from the OH-group of the datively bonded molecules to a Si surface atom. Despite this low conversion barrier, adsorption into the intermediate and further reaction via proton transfer were found to be largely decoupled.
采用分子束技术研究了甲醇和水在Si(001)上的反应动力学。确定了初始吸附概率s作为入射分子动能E和表面温度T的函数。对于甲醇和水，均观察到一个非活化反应通道；发现动力学由反应生成配位键合中间态决定。推导了从该中间体转化为最终态的低转化势垒。这归因于反应机理，该机理通过配位键合分子的OH基团向Si表面原子的质子转移进行。尽管转化势垒较低，但发现吸附到中间体以及通过质子转移的进一步反应在很大程度上是解耦的。
