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Insight into Key Parameters for Fabricating Stable Single-Atom Pt-Ni_x Alloy by Reduction Environment-Induced

Xin Xiao^1,2, Shibo Xi², Wenjie Zang³

¹School of Chemical Engineering, Sichuan University, No. 24 South Section 1, Yihuan Road, Chengdu, 610065, P. R. China.

|November 10, 2022

Summary

Researchers developed highly stable single-atom platinum catalysts using a novel anti-Ostwald approach. These catalysts show excellent performance in cellulose hydrogenolysis and are promising for green hydrogen production.

Keywords:

X-ray absorption cellulose hydrogenolysis nanocatalysts platinum

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Area of Science:

Catalysis
Materials Science
Green Chemistry

Background:

Developing stable single-atom catalysts is crucial for hydrogenation/dehydrogenation reactions and green hydrogen generation.
Existing catalysts often lack stability under harsh reduction conditions.

Purpose of the Study:

To synthesize highly stable single-atom platinum (Pt) catalysts using a reduction environment-induced anti-Ostwald approach.
To investigate the stabilization mechanism of single Pt atoms on a nickel-confined Al2O3 matrix.
To evaluate the catalytic performance in cellulose hydrogenolysis under demanding conditions.

Main Methods:

Synthesis of single-atom Pt catalysts on Al2O3 via a reduction environment-induced anti-Ostwald method.
In-situ X-ray absorption spectroscopy (XAS) to study electronic structure and bonding.
High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) for atomic-level imaging.
Density functional theory (DFT) simulations for validation.

Main Results:

Successfully achieved single-atom Pt catalysts (Pt-Nix) stabilized by metallic Ni clusters on an Al2O3 matrix.
In-situ XAS confirmed the formation of isolated Pt-Nix metallic bonds at high reduction temperatures, crucial for single Pt atom formation.
HAADF-STEM and DFT simulations validated that Ni clusters enhance Pt single-atom stability.
Demonstrated excellent catalytic performance in cellulose hydrogenolysis under harsh reductive and hydrothermal conditions.

Conclusions:

The developed single-atom Pt catalysts exhibit superior stability and performance, particularly in cellulose hydrogenolysis.
The anti-Ostwald approach combined with Ni confinement offers a viable strategy for creating robust single-atom catalysts.
These findings have broad implications for various hydrogen-involved reactions, including CO2 hydrogenation and green hydrogen production.