Graphdiyne Interface Engineering: Highly Active and Selective Ammonia Synthesis.

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• The electrochemical nitrogen reduction reaction (ECNRR) is a promising sustainable pathway for ammonia synthesis.
• Developing highly active and selective electrocatalysts remains a key challenge for efficient ECNRR.

Purpose of the Study:

• To fabricate a freestanding 3D graphdiyne-cobalt nitride (GDY/Co2N) electrocatalyst with an optimized interface for ECNRR.
• To investigate the electronic properties and catalytic performance of the novel GDY/Co2N material.

Main Methods:

• Fabrication of a 3D graphdiyne-cobalt nitride (GDY/Co2N) freestanding structure.
• Density functional theory (DFT) calculations to understand the electronic structure and bonding at the GDY/Co2N interface.
• Experimental electrochemical measurements to evaluate ammonia yield rate and Faradaic efficiency.

Main Results:

• The interface-bonded GDY imparts unique p-electronic character, enhancing the Co-N compound surface bonding.
• Achieved a record-breaking ammonia yield rate of 219.72 μg h⁻¹ mg⁻¹cat.
• Demonstrated a high Faradaic efficiency of 58.60% in acidic conditions.

Conclusions:

• The GDY/Co2N catalyst exhibits superior activity and selectivity for ECNRR due to optimized interface electronic properties.
• This work presents a promising new catalyst for sustainable ammonia production and advances the field of electrocatalysis.