Final Technical Report: First Principles Investigations for the Ensemble Effects of PdAu and PtAu Bimetallic Nanocatalysts

Ruqian Wu

关键词: CATALYSIS;    CATALYSTS;    CHEMICAL PROPERTIES;    DEHYDROGENATION;    ETHYLENE;    HETEROGENEOUS CATALYSIS;    METHANOL;    OXIDATION;    SHAPE;    SUBSTRATES;    WATER First Principles Investigations;    Ensemble Effects;    Bimetallic Nanocatalysts;   

DOI  :  10.2172/1040706
RP-ID  :  DOE/ER/15611-1 Final Report
PID  :  OSTI ID: 1040706
Others  :  TRN: US201212%%917

美国|英语

来源: SciTech Connect

【 摘 要 】

Bimetallic surfaces with tunable chemical properties have attracted broad attention in recent years due to their ample potential for heterogeneous catalysis applications. The local chemical properties of constituents are strongly altered from their parent metals by 'ligand effect', a term encompassing the influences of charge transfer, orbital rehybridization and lattice strain. In comparison to the aforementioned, the 'ensemble effect' associated with particular arrangements of the active constituents have received much less attention, despite their notable importance towards the determination of reactivity and selectivity of bimetallic catalysts. We performed theoretical studies for understanding the ensemble effects on bimetallic catalysis: (i) simulations for the formation of different ensembles on PdAu and PtAu nanoclusters; (ii) studies of the size, shape, and substrate dependence of their electronic properties; and (iii) simulations for model reactions such as CO oxidation, methanol, ethylene and water dehydrogenation on PdAu and PtAu nanoclusters. In close collaboration with leading experimental groups, our theoretical research elucidated the fundamentals of Au based bimetallic nanocatalysts.