Boosting Electrocatalytic N₂ Reduction to NH₃ over Two-Dimensional Gallium Selenide by Defect-Size Engineering

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Nitrogen reduction reaction (NRR) is crucial for sustainable ammonia production.
• Developing efficient electrocatalysts for NRR remains a significant challenge.
• Two-dimensional materials offer tunable electronic properties for catalysis.

Purpose of the Study:

• To investigate the potential of defective gallium selenide (V-GaSe) for nitrogen fixation and NRR.
• To explore the effect of defect size and strain on NRR performance.
• To design novel materials for enhanced NRR catalysis.

Main Methods:

• Density functional theory (DFT) calculations were employed.
• Simulations of pristine and strained V-GaSe and Janus V-GaInSe2 structures were performed.
• Analysis of N2 adsorption, reaction pathways, and onset potentials for NRR.

Main Results:

• Exposed Ga atoms in V-GaSe exhibit good N2 fixation capacity.
• Tensile strain enhances N2 adsorption and electrochemical NRR performance.
• Strained V-GaSe and V-GaInSe2 show low onset potentials (0.30 V and 0.31 V, respectively).
• Rapid removal of produced NH3 and suppressed hydrogen evolution reaction observed.

Conclusions:

• Defect-size-dependent tuning is a viable strategy for optimizing NRR catalysts.
• V-GaSe and related structures are promising for sustainable ammonia synthesis.
• This work provides new insights into N2 fixation mechanisms and catalyst design.