Gas binding to Au13, Au12Pd, and Au11Pd2 nanoclusters in the context of catalytic oxidation and reduction reactions.
Gas binding to Au13, Au12Pd, and Au11Pd2 nanoclusters in the context of catalytic oxidation and reduction reactions.
复制标题
在催化氧化和还原反应中气体与 Au13、Au12Pd 和 Au11Pd2 纳米团簇结合。
DOI：
--
复制
发表时间：
2008
影响因子：
4.4
通讯作者：
A. Chaffee
中科院分区：
文献类型：
--
作者：
B. A. Wells;A. Chaffee
通过原子中心密度泛函理论计算，研究了 Au(13)、Au(12)Pd 和 Au(11)Pd(2) 纳米团簇结合小分子碳氢化合物氧化和还原中常见物质的能力。已计算 CO(2)、H(2)、CO、O(2)、CH(4)、H(2)O、*O、*H、*CHO、*CO(2)H 和 *OH 的结合能。对于纯金纳米团簇，CO(2)、H(2)和CH(4)被发现不结合，O(2)和H(2)O以小于15 kcal mol(-1)的结合能弱结合，其余的以26-68 kcal mol(-1)范围内的结合能强结合。结合额外的气体分子并没有大大降低结合能。将钯添加到团簇中可以为所有测试气体创建结合位点。与钯原子的结合通常会增加分子的结合能，但会降低自由基的结合能。
The ability of Au(13), Au(12)Pd, and Au(11)Pd(2) nanoclusters to bind species typically found in the oxidation and reduction of small hydrocarbon has been investigated by means of atom centered density functional theory calculations. Binding energies of CO(2), H(2), CO, O(2), CH(4), H(2)O, *O, *H, *CHO, *CO(2)H, and *OH have been calculated. For pure gold nanoclusters, CO(2), H(2), and CH(4) were found to not bind, and O(2) and H(2)O bound weakly with binding energies less than 15 kcal mol(-1), with the rest binding strongly with binding energies in the range 26-68 kcal mol(-1). Binding additional gas molecules did not greatly reduce the binding energy. Adding palladium to the clusters created binding sites for all of the test gases. Binding to the palladium atom generally increased the binding energy of molecules but decreased the binding energy of radicals.