Pore-Space-Partition-Oriented Sandwich Platinum Array Confined in a Metal-Organic Framework for Boosting Overall...

Area of Science:

• Materials Science
• Nanotechnology
• Catalysis

Background:

• Atomic-level dispersion of noble metals in porous materials is key for efficient catalysts but remains challenging.
• Current methods struggle to control metal atom distribution and electronic properties within catalytic frameworks.

Purpose of the Study:

• To develop a method for precisely confining platinum (Pt) atoms within a metal-organic framework (MOF) to create highly efficient and stable electrocatalysts.
• To investigate the relationship between pore structure, Pt atom arrangement, and catalytic activity.

Main Methods:

• Inspired by sandwich compounds, Pt atoms were confined in MOFs using pore space partition via conjugate interactions with aromatic pore partitioners.
• AC high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray absorption spectroscopy (XAS), and theoretical simulations were employed.
• The distance between aromatic rings was systematically varied to control Pt particle size and electronic structure.

Main Results:

• Formation of 1D infinite Pt arrays within the MOF structure.
• A linear decrease in Pt particle size with decreasing aromatic ring distance, correlating with electronic orbital regulation.
• The optimized Pt@MOF-BCP catalyst exhibited highly efficient Pt utilization, superior electron transmission, and excellent stability.
• Ultratow overpotentials for hydrogen evolution reaction (HER) (2.5 mV) and oxygen evolution reaction (OER) (265 mV) at 10 mA·cm^-2.
• A reduced cell voltage of 1.47 V at 10 mA·cm^-2 in practical applications.

Conclusions:

• The developed method enables precise control over atomic-level Pt dispersion in MOFs, leading to advanced electrocatalytic materials.
• Pt@MOF-BCP demonstrates exceptional difunctional electrocatalytic performance, surpassing most benchmark catalysts.
• This approach offers a promising pathway for designing next-generation catalysts with enhanced efficiency and stability.