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Arrayed Pt Single Atoms via Phosphotungstic Acids Intercalated in Silicate Nanochannels for Efficient Hydrogen
Je-Wei Chang1,2, Kuan-Hsuan Su3, Chih-Wen Pao2
1Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan.
ACS Nano
|January 3, 2024
Summary
Arrayed single platinum (Pt) atoms were synthesized using phosphotungstic acid (PTA) within silicate nanochannels. This novel method enhances Pt single-atom loading and catalytic efficiency for hydrogen production.
Area of Science:
- Materials Science
- Catalysis
- Nanotechnology
Background:
- Single-atom catalysts (SACs) exhibit high activity but are typically randomly distributed on 2D substrates.
- Developing methods for controlled synthesis and high loading of SACs is crucial for advanced applications.
Purpose of the Study:
- To develop a strategy for preparing arrayed single Pt atoms with high loading.
- To investigate the stabilization mechanism and control over Pt atom dispersion.
- To evaluate the catalytic performance of the arrayed single-atom catalyst for hydrogen production.
Main Methods:
- Templated synthesis of arrayed single Pt atoms using phosphotungstic acid (PTA) within hexagonally packed silicate nanochannels.
- Characterization using X-ray absorption spectroscopy (XAS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and energy-dispersive X-ray spectroscopy (EDS).
- Density-functional theory (DFT) calculations to understand Pt atom stabilization and clustering behavior.
Main Results:
- Achieved high single Pt-atom loading (ca. 3.0 wt %) through coordination with intercalated PTA within silicate nanochannels.
- Confirmed stabilization of single Pt atoms via four-oxygen coordination with PTA on the nanochannel walls.
- Demonstrated control over Pt atom dispersion versus clustering by adjusting the PTA density.
- Achieved a hydrogen production rate of ca. 300 mmol/h/gPt, approximately double the efficiency of previous Pt-based photocatalytic systems.
Conclusions:
- A novel strategy for fabricating arrayed single Pt atoms within silicate nanochannels using PTA as a template was successfully developed.
- The interaction between PTA and the silicate substrate is key to reducing Pt adsorption energy and preventing clustering.
- The 3D organized Pt single-atom catalyst exhibits significantly enhanced and stable efficiency for hydrogen production, offering a promising avenue for photocatalysis.
