Laboratoire de Dynamique, Interactions et Réactivité, Université Pierre et Marie Curie-Paris 6, CNRS, UMR 7075, Case Courrier 49, Bat F 74, 4 Place Jussieu, 75252 Paris Cedex 05, France.
J Phys Chem A. 2010 Mar 11;114(9):3320-8. doi: 10.1021/jp909600q.
The successive hydrogenation of CO has been investigated by two methods. The first is hydrogenation of a CO surface. The second is co-injection of CO molecules and H atoms. Both methods have been performed at 3 and 10 K. In the first method, the interaction of H atoms with solid CO at 10 K shows that CO is consumed to form H(2)CO and CH(3)OH. No trace of species such as HCO and CH(3)O is detected. No product was observed when the same experiment was performed at 3 K. In the second method, when H and CO are codeposited at 10 K, HCO and CH(3)O are observed. In fact, the yield of these intermediate species depends on the amount of the H radicals interacting with CO molecules. At 3 K, the presence of H(2) in the solid screens the hydrogenation reaction. This causes a termination for the reaction in the stage of the formation of HCO and H(2)CO. At 10 K, H(2) cannot condense, and the reaction between CO and H is total. In this case, species such as HCO, H(2)CO, CH(3)O, and CH(3)OH are observed.
已通过两种方法研究了 CO 的连续加氢。第一种是 CO 表面的加氢。第二种是 CO 分子和 H 原子的共注入。这两种方法都在 3 和 10 K 下进行。在第一种方法中,H 原子与 10 K 下的固态 CO 的相互作用表明 CO 被消耗形成 H(2)CO 和 CH(3)OH。没有检测到 HCO 和 CH(3)O 等物质的痕迹。当在 3 K 下进行相同的实验时,没有观察到产物。在第二种方法中,当 H 和 CO 在 10 K 下共沉积时,观察到 HCO 和 CH(3)O。事实上,这些中间物种的产率取决于与 CO 分子相互作用的 H 自由基的数量。在 3 K 下,固态中的 H(2)会屏蔽加氢反应。这导致反应在 HCO 和 H(2)CO 的形成阶段终止。在 10 K 下,H(2)不能冷凝,并且 CO 和 H 之间的反应是完全的。在这种情况下,观察到 HCO、H(2)CO、CH(3)O 和 CH(3)OH 等物质。