Phases and Architectures in Metal/Metal Oxide Systems Driven by Strong Metal-Support Interactions

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Metal oxide supported metal catalysts are crucial for industrial applications.
• Strong metal-support interaction (SMSI) describes dynamic structural changes under reducing atmospheres, affecting catalyst performance.
• Experimental monitoring of SMSI interfaces is challenging due to complex compositional and structural variations.

Purpose of the Study:

• To computationally investigate the atomic-level structure and phase diversity of metal/metal oxide interfaces under SMSI conditions.
• To understand the factors governing the formation of different phases and the electronic properties of SMSI materials.
• To develop descriptors for predicting and controlling SMSI behavior in catalyst design.

Main Methods:

• Density functional theory (DFT) calculations.
• Machine learning interatomic potentials (MLIPs).
• Global minima structure searching algorithms.
• Systematic construction of interfaces between common catalytic metals (Ni, Pd, Pt) and reducible metal oxides (r-TiO2, CeO2, In2O3).

Main Results:

• Identified phase diversity driven by competition between alloy and oxide formation.
• Demonstrated that local suboxide layer properties dictate the final architecture, composition, and electronic properties.
• Proposed two descriptors to explain the observed phase diversity in SMSI systems.
• Provided atomic-level insights into the complex metal/metal oxide interfaces.

Conclusions:

• The study offers a systematic computational approach to understanding SMSI phenomena.
• The findings advance the rational design of SMSI-based catalytic materials.
• Insights into atomic-level interface architecture are crucial for optimizing catalytic performance.