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Energetics of Nanoparticle Exsolution from Perovskite Oxides
Yang Gao1,2, Ziheng Lu1, Tsam Lung You1
1Department of Mechanical and Aerospace Engineering , The Hong Kong University of Science and Technology , Hong Kong , SAR, China.
In situ exsolution of nickel nanoparticles on perovskite oxides enhances electrochemical performance. Surface vacancies and termination significantly influence nickel migration and nanoparticle formation, leading to improved stability and activity.
Area of Science:
- Materials Science
- Electrochemistry
- Computational Chemistry
Background:
- Active metal nanoparticles boost electrochemical performance in ABO3 perovskite oxides.
- In situ exsolution offers superior nanoparticle stability compared to conventional deposition methods.
Purpose of the Study:
- Investigate the energetics of transition metal atom migration during in situ exsolution.
- Understand the influence of surface orientation and composition on nanoparticle formation in SrTiO3.
Main Methods:
- Utilized ab initio computations to model surface energetics.
- Employed experimental studies using a SrTiO3-based model system.
Main Results:
- Calculations revealed preferential Ni segregation to (100)-oriented, SrTiO-terminated surfaces.
- Sr-site and O-site vacancies promoted Ni segregation, while La doping inhibited it.
- Experiments confirmed computational predictions, showing enhanced activity with Sr vacancies and no La.
Conclusions:
- Surface vacancies and termination critically control in situ nanoparticle exsolution in perovskite oxides.
- The developed approach can guide the design of new materials for enhanced catalytic activity and stability.
- This study provides a mechanistic understanding for optimizing nanoparticle exsolution processes.
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