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Encapsulating Metal Nanoparticles into a Layered Zeolite Precursor with Surface Silanol Nests Enhances Sintering
Ang Li1, Yuyan Zhang1, Christopher J Heard1
1Department of Physical and Macromolecular Chemistry, Faculty of Science, Charles University, Hlavova 8, 128 43, Prague 2, Czech Republic.
Angewandte Chemie (International Ed. in English)
|November 7, 2022
Summary
This study introduces a new method to stabilize ultra-small rhodium (Rh) nanoparticles using a layered zeolite (IPC-1P), preventing high-temperature deactivation and enhancing catalytic activity.
Area of Science:
- Materials Science
- Catalysis
- Nanotechnology
Background:
- Supported metal nanoparticles are crucial heterogeneous catalysts but suffer from sintering and deactivation at high temperatures.
- Existing porous supports offer limited additional stabilization for metal nanoparticles.
- Zeolites, particularly layered silanol-rich structures, present an opportunity for enhanced nanoparticle stabilization.
Purpose of the Study:
- To stabilize ultra-small rhodium (Rh) nanoparticles within a silanol-rich layered zeolite (IPC-1P) to prevent sintering.
- To investigate the effect of adjusting interlayer spacing in IPC-1P on nanoparticle architecture and stability.
- To develop a novel, catalytically active material by combining zeolite confinement and metal-silanol interactions.
Main Methods:
- Utilized the layered zeolite IPC-1P as a support for ultra-small Rh nanoparticles.
- Adjusted IPC-1P interlayer spacing via swelling to create various porous architectures (microporous, mesoporous).
- Employed in situ scanning transmission electron microscopy (STEM) to observe nanoparticle behavior at high temperatures.
- Performed density functional theory (DFT) calculations to understand metal-silanol interactions and migration barriers.
Main Results:
- Rh nanoparticles confined within IPC-1P demonstrated remarkable resistance to sintering at 750°C for 6 hours.
- Rh clusters exhibited strong binding to surface silanol quadruplets within the zeolite layers via hydrogen transfer.
- High silanol density within IPC-1P was computationally shown to hinder nanoparticle migration.
- A novel, catalytically active material, Rh@IPC_C22, was successfully synthesized by combining swelling, surfactant treatment, and metal-silanol interactions.
Conclusions:
- The silanol-rich layered zeolite IPC-1P effectively stabilizes ultra-small Rh nanoparticles against high-temperature sintering.
- Metal-silanol interactions, facilitated by hydrogen transfer and hindered migration, are key to the observed stability.
- The developed Rh@IPC_C22 material represents a promising advancement in heterogeneous catalysis due to its enhanced stability and activity.
