Local environmental engineering for highly stable single-atom Pt₁/CeO₂catalysts: first-principles insights

Area of Science:

• Materials Science
• Catalysis
• Electrochemistry

Background:

• Single-atom catalysts offer potential solutions to cost and durability challenges in fuel cell electrocatalysts.
• Platinum-based catalysts are critical for fuel cell performance but face economic and stability limitations.

Purpose of the Study:

• To systematically investigate the stability and interaction mechanisms of single-atom platinum on cerium dioxide (Pt₁/CeO₂) systems.
• To understand the fundamental principles governing the stability of Pt₁/CeO₂ for fuel cell applications.

Main Methods:

• Utilized first-principles calculations to model and analyze the Pt₁/CeO₂ system.
• Decomposed Pt adsorption energy into chemical interaction and surface deformation components.
• Investigated the role of local chemical environment and electronic metal-support interactions.

Main Results:

• Identified Pt-O bond formation as the primary factor determining Pt₁/CeO₂ stability.
• Determined that a Pt-4O configuration leads to the highest stability with Pt oxidized to Pt²⁺.
• Confirmed the dynamic stability of the Pt₁/CeO₂(100) surface and the influence of the oxygen environment on Pt oxidation states.

Conclusions:

• Proposed an electronic metal-support interaction mechanism to explain the observed stability of Pt₁/CeO₂.
• External oxygen can further oxidize platinum, enhancing catalyst properties (Ptⁿ⁺, 2 ≤ n < 4).
• Findings provide critical guidance for designing highly stable and efficient electrocatalysts for fuel cells.