Electronic Modulation and Active Site Exposure Using C₆₀ Fullerenolamine Enable High-Performance Alcohol Oxidation on...

Area of Science:

• Materials Science
• Catalysis
• Electrochemistry

Background:

• Catalyst performance relies on active site availability and electronic structure.
• Metal heterogeneous catalysts are vital for many chemical reactions, including alcohol oxidation.

Purpose of the Study:

• To develop and evaluate a novel C60 fullerenolamine (FA)-modified Pd metallene (Pdene) catalyst system.
• To investigate the role of FA in enhancing Pdene's catalytic activity and stability for alcohol oxidation.

Main Methods:

• Synthesis of FA-modified Pdene catalyst.
• Electrochemical characterization to assess active surface area and catalytic performance.
• In-situ Fourier transform infrared spectroscopy and density functional theory calculations for mechanistic studies.

Main Results:

• FA modification increased electrochemical active surface area and induced an electron-deficient Pdene surface.
• Achieved a 54.5% increase in mass activity and 46.3% enhancement in specific activity for ethanol oxidation.
• Demonstrated superior operational stability, CO poisoning resistance, and C1 pathway selectivity.

Conclusions:

• FA-Pdene is an efficient catalyst system for alcohol oxidation, offering enhanced activity and stability.
• The fullerene ligand effectively modulates catalyst electronic properties and active site availability.
• This fullerene-mediated catalytic approach shows promise for advancing metal-based catalytic systems.