Augmented Electrochemical Oxygen Evolution by d-p Orbital Electron Coupling.

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• High-entropy materials, including alloys, oxides, and hydroxides, show promise for electrocatalysis but suffer from activity deficiencies.
• Tailoring structure-activity relationships in multicomponent systems is crucial for advancing electrocatalytic performance.

Purpose of the Study:

• To develop a novel high-entropy material for efficient oxygen evolution reaction (OER) electrocatalysis.
• To investigate the structure-activity relationship and performance enhancement mechanisms in high-entropy systems.

Main Methods:

• Fabrication of a 2D high-entropy metal phosphorus trisulfide, specifically (MnFeCoNiZn)PS3.
• Electrocatalytic performance testing for OER, including overpotential, Tafel slope, and long-term stability measurements.
• Density functional theory (DFT) calculations to elucidate the electronic structure and catalytic mechanisms.

Main Results:

• The (MnFeCoNiZn)PS3 material exhibited excellent OER activity with a low overpotential of 240 mV at 10 mA cm⁻² and a minimal Tafel slope of 32 mV dec⁻¹.
• The catalyst demonstrated remarkable stability, with negligible degradation over 96 hours of operation under varying current densities.
• DFT calculations revealed that d-p orbital hybridization and the contribution of active phosphorus centers enhance catalytic performance.

Conclusions:

• Entropy-driven composition engineering in high-entropy anion-regulated transition metal compounds is an effective strategy for designing advanced OER electrocatalysts.
• The developed 2D high-entropy metal phosphorus trisulfide provides a versatile platform for optimizing electron coordination environments and improving catalytic efficiency.
• This work offers a promising approach for developing next-generation catalysts for energy-related applications.