High-selectivity electrocatalytic ammonia oxidation on Mo single-atom catalysts supported on BP@ZrC

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical ammonia oxidation efficiency is limited by poor selectivity.
• Current catalysts lack detailed structure-activity relationship studies.
• Developing selective catalysts is crucial for ammonia oxidation.

Purpose of the Study:

• To design and investigate transition metal single-atom catalysts on BP@ZrC substrates for electrochemical ammonia oxidation.
• To understand the structure-activity relationship and optimize catalyst performance.
• To identify high-performance catalysts with enhanced selectivity and low overpotential.

Main Methods:

• Density functional theory (DFT) calculations were employed.
• Systematic investigation of thermodynamic stability and catalytic activity.
• Analysis of electronic structure and reaction mechanisms.

Main Results:

• The designed single-atom catalysts effectively suppressed the nitrogen-oxygen coupling side reaction.
• Mo-BP@ZrC was identified as the optimal catalyst with a low overpotential of 0.49 V.
• 100% selectivity for N2 production was achieved, with NH2* activation mechanism elucidated.

Conclusions:

• A clear structure-activity relationship was established for designing electrochemical ammonia oxidation catalysts.
• The study provides high-performance candidate catalysts and a theoretical foundation for efficient catalyst development.
• Mo-BP@ZrC offers a promising pathway for selective electrochemical ammonia oxidation.