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Single-Atom-Layer-Induced Reversed Diffusion Pathway of Reactive Metal-Support Interaction.
Xiao Han1, Shuwen Niu2, Geng Wu3
1Hefei National Research Center for Physical Sciences at the Microscale, Department of Applied Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, P.R. China.
Journal of the American Chemical Society
|November 27, 2025
Summary
This study reveals a new mechanism for reactive metal-support interaction (RMSI) in Pt/TiO2 catalysts. Platinum atoms first form a single layer on the support before titanium incorporates, creating an efficient intermetallic compound for catalysis.
Area of Science:
- Catalysis science
- Materials science
- Surface chemistry
Background:
- Reactive metal-support interaction (RMSI) is crucial for tuning catalyst properties.
- Existing models propose metal atom diffusion from support to nanoparticles during RMSI.
Purpose of the Study:
- To elucidate the atomic-level mechanism of RMSI in Pt/TiO2 catalysts.
- To investigate the formation pathway of platinum-titanium intermetallic compounds (IMCs).
Main Methods:
- In situ heating aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM).
- Theoretical analysis of diffusion pathways and electronic structure changes.
Main Results:
- A reversed diffusion pathway for RMSI was observed, with Pt atoms spreading to form a single-atom layer on TiO2 first.
- This single-atom layer Pt facilitated Ti-O bond weakening, oxygen release, and Ti migration, enabling Pt3Ti IMC formation.
- The resulting Pt3Ti IMC showed electron-rich Pt sites and enhanced resistance to CO poisoning.
Conclusions:
- The formation of a single-atom-layer Pt intermediate is key to effective IMC formation in Pt/TiO2.
- Understanding this reversed diffusion pathway provides guidance for designing catalysts with improved IMC formation and performance.
- The Pt3Ti IMC demonstrates superior electrocatalytic activity for hydrogen oxidation due to reduced CO poisoning.
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