Structural Rearrangement of Au–Pd Nanoparticles under Reaction Conditions: An ab Initio Molecular Dynamics Study
The structure, composition, and atomic distribution of nanoalloys under operating conditions are of significant importance for their catalytic activity. In the present work, ab initio molecular dynamics simulations are performed to understand the structural behavior of a Au-Pd nanoalloy supported on rutile TiO2 under different conditions. We find that the Au-Pd structure is strongly dependent on the redox properties of the support, originating from strong metal-support interactions. Under reducing conditions, Pd atoms are inclined to move toward the metal/oxide interface, evidenced by a significant increase of Pd-Ti bonds. This could be attributed to the charge localization at the interface that leads to Coulomb attractions to positively charged Pd atoms. In contrast, Pd atoms would rather stay inside the nanoparticle or on the alloy surface under oxidizing conditions. Moreover, Pd atoms on can be stabilized by hydrogen adsorption, forming Pd-H bonds, which are stronger than Au-H bonds. Our work provides an important insight into the structure design of Pd-Au nanoalloy catalyst and may lead to potential applications in dioxygen activation processes where Pd atoms are generally considered to be the active sites.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1479097
- Report Number(s):
- PNNL-SA-122190
- Journal Information:
- ACS Nano, Vol. 11, Issue 2; ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
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