Revealing Dynamics and Competitive Mechanism of Gas-Induced Surface Segregation of PdFe<sub>0.08</sub> Dilute Alloy by Multi-Dimensional Imaging
The restructuring of dilute alloys under gas environments has shown a great impact on their catalytic performance due to intriguing structural sensitivity, but the structural dynamics and underlying mechanism remains elusive. Herein, we directly resolved the distinct dynamic behaviors of PdFe<sub>0.08</sub> dilute alloys under CO or O<sub>2</sub> environment by multidimensional imaging. The stronger binding of gaseous CO with Fe atoms stimulates Fe segregation out of the PdFe<sub>0.08</sub>, resulting in 3D growth of Fe islands, whereas the dissociative adsorption of O<sub>2</sub> results in 2D layer-by-layer growth of segregated FeO as encapsulation overlayers that bind strongly with the Pd surface underneath. Such varied structures remarkably tune the catalytic activity for CO oxidation, showing a considerably high activity for a CO-treated sample. Our results reveal the competitive mechanism between adsorbate-metal and metal-metal interaction for gas-induced surface segregation, which should be highly considered for the rational design of dilute alloys with dynamically tuned structure and reactivity.
Authors
- Yangsheng Li (ORCID: https://orcid.org/0000-0001-7289-5278)
- Jinming Cai (ORCID: https://orcid.org/0000-0003-0869-1515)
- Yong Zhang (ORCID: https://orcid.org/0000-0002-3284-2865)
- Junling Lu (ORCID: https://orcid.org/0000-0002-2607-6869)
- Tao Zhang (ORCID: https://orcid.org/0000-0001-9470-7215)
- Fang Liu (ORCID: https://orcid.org/0000-0001-5759-3511)
- Bing Yang (ORCID: https://orcid.org/0000-0003-3515-0642)
- Yafeng Zhang (ORCID: https://orcid.org/0000-0003-0209-8163)
- Hong Li
- Fan Yang (ORCID: https://orcid.org/0000-0002-1406-9717)
- Mengwei Li (ORCID: https://orcid.org/0000-0001-6163-2827)
- Feng Yin (ORCID: https://orcid.org/0000-0003-1785-8831)
Institutions
- Kunming University of Science and Technology (CN)
- University of Science and Technology of China (CN)
- Dalian Institute of Chemical Physics (CN)
- Chinese Academy of Sciences (CN)
- ShanghaiTech University (CN)
- Shaanxi Normal University (CN)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2024-11-15
- DOI
- https://doi.org/10.1021/acs.jpclett.4c02903
- Citations
- 1
- Primary Topic
- nanoparticles nucleation surface interactions
- Type
- article
- Field-Weighted Citation Impact
- 0.38
Funders
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- China Postdoctoral Science Foundation
- Dalian Institute of Chemical Physics
- National Key Research and Development Program of China