A single-atom potential confinement strategy for stabilizing rhodium nanocatalysts in methane oxidation
Chenxin Xu1, Zhi-Qiang Wang2, Tian Qin3
1Department of Environmental Science & Engineering, Fudan University, Shanghai, China.
Stabilizing rhodium (Rh) nanocatalysts under harsh conditions is crucial. Pre-anchoring guest atoms creates a confinement field, preventing Rh nanoparticle degradation and maintaining high activity during methane oxidation.
Area of Science:
- Materials Science
- Catalysis
- Surface Chemistry
Background:
- Nanometal catalysts often deactivate under harsh conditions due to disintegration into less active single atoms or clusters.
- This degradation leads to loss of active components and reduced catalytic efficiency.
Purpose of the Study:
- To develop a strategy for stabilizing rhodium (Rh) nanocatalysts on ceria (CeO₂) supports under severe reaction conditions.
- To investigate the mechanism of catalyst stabilization and its impact on methane oxidation activity.
Main Methods:
- Theoretical calculations (Density Functional Theory) to study atom anchoring energetics on CeO₂.
- Synthesis of Rh nanocatalysts with and without pre-anchored guest atoms on CeO₂.
- Catalytic testing for methane oxidation under simulated engine conditions.
- Environmental scanning transmission electron microscopy (STEM) for structural characterization before and after high-temperature aging.
Main Results:
- Pre-filling surface vacancies with guest atoms energetically hinders subsequent Rh anchoring, creating a confinement effect.
- Single-atom-confined Rh nanocatalysts retained structural integrity and high activity after aging at 800°C, unlike unprotected catalysts.
- Unprotected Rh catalysts degraded into single atoms, losing low-temperature reactivity.
- Low-temperature methane oxidation activity was attributed to delocalized electrons in Rh nanoparticles, not Rh-CeO₂ single-atom interactions.
Conclusions:
- A novel energy confinement strategy effectively stabilizes supported Rh nanocatalysts against degradation under harsh conditions.
- This approach maintains high catalytic activity, particularly for low-temperature methane oxidation.
- The findings offer a new paradigm for designing robust nanocatalysts beyond conventional metal-support interactions.
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