| AVS 65th International Symposium & Exhibition | |
| Fundamental Discoveries in Heterogeneous Catalysis Focus Topic | Tuesday Sessions |
| Session HC+SS-TuM |
| Session: | Nanochemistry in Heterogeneous Catalysis |
| Presenter: | Tao Jiang, University of Central Florida |
| Authors: | T. Jiang, University of Central Florida T.B. Rawal, Oak Ridge National Laboratory D. Le, University of Central Florida T.S. Rahman, University of Central Florida |
| Correspondent: | Click to Email |
The rational design of single metal atoms anchored on non-metallic surface has the great potential to offer catalysts with high activity and selectivity [1]. Towards this goal, we have carried out density functional theory based calculations of the catalytic behavior of singly dispersed Pt atoms on ZnO, Pt1/ZnO(10-10), as a model system for methanol partial oxidation. We find that methanol adsorption is favored at the surface Zn site whereas oxygen prefers to adsorb at the Pt-Zn site. The adsorption of reaction intermediates CO, CO2, and H2 are favored at the Pt site, whereas H2O prefers to sit at the Zn site. Secondly, along the reaction pathways for methanol dehydrogenation, we will illustrate that the O-H bond scission from methanol is slightly exothermic (ΔE=-13 meV). The resultant methoxy then preferentially adsorbs at the Pt-Zn site, where C-H bond of methoxy can be easily activated. The dissociation of methoxy (CH3O->CH2O+H) is exothermic (ΔE=-0.42 eV) and that of formaldehyde (CH2O->CHO+H) is endothermic (ΔE=+0.16 eV). The results suggest that Pt1/ZnO(10-10) is a potential single-atom catalyst for methanol oxidation. We will compare our findings with those for the related system Pd1/ZnO(10-10) [1] and available experimental observations to evaluate their relative advantages for methanol partial oxidation.
[1] T. B. Rawal, S. R. Acharya, S. Hong, D. Le, Y. Tang, F. F. Tao, and T. S. Rahman, submitted (2018).
The work is partially supported by DOE grants DE-FG02-07ER15842