Rh1/-Al2O3 Single-Atom Catalysis of O2 Activation and CO Oxidation: Mechanism, Effects of Hydration, Oxidation State, and Cluster Size
Rh1/-Al2O3 Single-Atom Catalysis of O2 Activation and CO Oxidation: Mechanism, Effects of Hydration, Oxidation State, and Cluster Size
复制标题
DOI：
10.1002/cctc.201200799
复制
发表时间：
2013-07-01
期刊：
影响因子：
4.5
通讯作者：
Nair, Nisanth N.
中科院分区：
文献类型：
--
作者：
Ghosh, Tushar K.;Nair, Nisanth N.
本文采用从头算分子动力学方法研究了Rh_1/-Al_2 O_3单原子催化O_2活化和CO氧化反应。我们仔细研究的完整的催化循环，涉及连续两个CO分子的氧化机制的分子细节。Rh的表面水合和氧化态对O2活化和CO氧化动力学的影响。我们还报告在这里的催化活性的实验拦截RhI（CO）2上-Al 2 O 3。此外，我们描绘的重要性，通过比较的Rh 6/Al 2 O3催化剂的性能的单原子催化。一个分子水平上的理解的差分反应的水合，氧化，和一个较大的Rh簇大小的报告。
The single-atom catalysis of O2 activation and CO oxidation with Rh1 supported on -Al2O3 is investigated here through abinitio molecular dynamics techniques. We scrutinize the molecular details of the mechanism for the full catalytic cycle that involves the oxidation of two CO molecules in succession. The effect of the surface hydration and oxidation state of Rh on the kinetics of O2 activation and CO oxidation is presented. We also report here the catalytic activity of experimentally intercepted RhI(CO)2 on -Al2O3. Furthermore, we delineate the importance of single-atom catalysis by comparing the performance of the Rh6/Al2O3 catalyst. A molecular level understanding of the differential reactivity on hydration, on oxidation, and of a larger Rh cluster size is reported.