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Published on: June 21, 2017
Electro-chemo-mechanically Driven Ni Exsolution from (Pr,Ce,Ni)O2-δ: Controlled Nucleation Density and Enhanced
Sipei Zhang1,2, Lin Lin3, Yaguang Zhu3
1Department of Materials Science & Engineering, The Grainger College of Engineering, University of Illinois, Urbana-Champaign, 1304 West Green Street, Urbana, Illinois 61801, United States.
Facile exsolution of nickel nanoparticles from (Pr,Ce)O2-δ supports, driven by electrochemical potential, enhances electrocatalyst performance. This method boosts surface exchange for potential all-ceria electrochemical cells.
Area of Science:
- Materials Science
- Electrochemistry
- Nanotechnology
Background:
- In situ exsolution of metal nanoparticles is key for advanced electrocatalysts.
- High nanoparticle nucleation density under mild conditions is crucial for electrode performance.
- Fluorite-structured oxides offer potential as host lattices for nanoparticle exsolution.
Purpose of the Study:
- To demonstrate facile exsolution of nickel (Ni) nanoparticles from fluorite-structured (Pr,Ce)O2-δ.
- To investigate the impact of electrochemical potential on Ni nucleation density.
- To evaluate the electrochemical performance of Ni-exsolved catalysts.
Main Methods:
- Pulsed laser deposition to prepare (Pr,Ce,Ni)O2-δ thin films on YSZ substrates.
- High-throughput electrochemical cell with a Nernst voltage gradient.
- In situ synchrotron X-ray photoelectron spectroscopy and ex situ atomic force microscopy.
- Electrochemical impedance spectroscopy under reducing conditions.
Main Results:
- Nickel nanoparticles were successfully exsolved at 550 °C under cathodic bias.
- Nucleation density increased with electrochemical driving force (decreasing oxygen potential).
- The surface exchange coefficient of Ni-exsolved (Pr,Ce)O2-δ was ~4x higher than without exsolution.
Conclusions:
- Mixed-conducting fluorites are effective hosts for transition-metal exsolution.
- Electrochemical potential is a viable driving force for controlling nanoparticle exsolution.
- This approach enables the development of all-ceria electrochemical cells using (Pr,Ce)O2-δ as both cathode and anode.
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