Interfacial π-p Electron Coupling Prompts Hydrogen Evolution Reaction Activity in Acidic Electrolyte

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• 2H-phase Molybdenum Disulfide (MoS₂) shows promise for hydrogen evolution reaction (HER) due to favorable hydrogen adsorption energy.
• However, the inherent limitations of 2H-MoS₂ restrict its electrocatalytic efficiency for HER.

Purpose of the Study:

• To develop robust HER electrocatalysts by covalently bridging 2H-MoS₂ with graphitic carbon nitride (GCN).
• To investigate the mechanism of enhanced HER activity through π-p electron coupling at the MoS₂/GCN interface.

Main Methods:

• Synthesis of MoS₂/GCN composite material.
• Electrocatalytic testing for HER activity and durability.
• Density Functional Theory (DFT) calculations to elucidate electronic structure and reaction mechanisms.

Main Results:

• MoS₂/GCN demonstrated remarkable HER activity, achieving 160 mV at 10 mA·cm^-2.
• The composite exhibited excellent long-term durability.
• DFT calculations confirmed that π-p electron coupling at the interface enhances HER performance by regulating the electronic structure of sulfur atoms.

Conclusions:

• The MoS₂/GCN composite serves as a highly effective electrocatalyst for HER.
• The π-p electron coupling mechanism is crucial for boosting catalytic performance.
• This research offers a viable strategy for designing advanced electrocatalysts for energy conversion applications.