High-Entropy Oxide-Derived Graphdiyne: Exploiting Lattice Distortion and Oxygen Vacancies for Robust Photocatalytic...

Area of Science:

• Materials Science
• Nanotechnology
• Renewable Energy

Background:

• Graphdiyne (GDY) is a novel 2D carbon allotrope with potential in photocatalysis.
• Existing GDY applications are limited by poor stability on conventional substrates like copper.
• Developing stable and efficient GDY-based photocatalysts is crucial for hydrogen generation.

Purpose of the Study:

• To improve the efficacy and durability of graphdiyne (GDY) for photocatalytic hydrogen generation.
• To develop a novel HEO-GDY composite by replacing copper substrates with high-entropy oxide (HEO).
• To construct and evaluate a ZHG-10 photocatalyst integrating HEO-GDY with Zn_0.5Cd_0.5S.

Main Methods:

• Fabrication of HEO-GDY composite and ZHG-10 photocatalyst.
• Photocatalytic hydrogen evolution activity measurements.
• Photoelectrochemical tests, Kelvin probe force microscopy (KPFM), and density functional theory (DFT) calculations.

Main Results:

• The ZHG-10 photocatalyst achieved a hydrogen production rate of 7.59 mmol/g/h, outperforming GDY catalysts on copper.
• HEO-GDY demonstrated superior cycling stability compared to conventional GDY-based catalysts.
• HEO significantly enhanced charge carrier separation efficiency and introduced defective active sites.

Conclusions:

• The HEO-GDY composite offers enhanced stability and photocatalytic activity for hydrogen generation.
• Multi-metal synergy and lattice distortion in HEO create active sites for hydrogen adsorption and activation.
• This research presents a new strategy for high-performance, durable GDY-based photocatalytic systems.