4.8 Article

Mechanistic Insights into the Synthesis of Platinum-Rare Earth Metal Nanoalloys by a Solid-State Chemical Route

Journal

CHEMISTRY OF MATERIALS
Volume 33, Issue 2, Pages 535-546

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c03291

Keywords

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Funding

  1. DTU Energy TT project [49805]
  2. Danish ForskEL program (UPCAT) [2015-1-12315]
  3. Innovation Fund Denmark (4M Centre) [12-132710]
  4. DTU PoC Fond [48373, 49696]

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This study presents a comprehensive understanding of the synthesis mechanism of platinum-rare earth metal (Pt-RE) nanoalloys, achieved through systematic investigations of the chemical processes at different stages and the evolution of intermediate products. This paves the way for optimizing synthesis procedures and manipulating the method to synthesize Pt-RE alloy materials with desired structures and properties.
Platinum-rare earth metal (Pt-RE) nanoalloys are among the most active electrocatalysts for the oxygen reduction reaction and are predicted to exhibit long-term stability in proton-exchange membrane fuel cells. We have recently developed a solidstate chemical route for synthesizing this family of alloy materials, which is carried out under seemingly impossible conditions. Here, we report an in-depth understanding of the synthesis mechanism, obtained through systematic investigations of the chemical processes involved at different stages of the synthesis process and the structural evolution of the intermediate products. The formation of Pt-RE nanoalloys is made possible by a series of consecutive chemical and physical processes, including the polymerization processes of the nitrogen-rich precursor, the formation of a porous RE carbodiimide phase, the mobility of the formed metal phases on the carbon support, the reduction of the RE metals driven by the alloying reaction, and so forth. This thorough understanding of the mechanism of the synthesis process lays the foundation for optimizing the synthesis procedures and maneuvering this method to synthesize Pt-RE alloy materials with the desired structures and properties.

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