Biomimetic Elastic Single-Atom Protrusions Enhance Ammonia Electrosynthesis

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Electrocatalytic nitrogen (N₂) reduction reaction (eNRR) offers a sustainable pathway for ammonia (NH₃) production.
• Sluggish reaction kinetics currently limit the efficiency of eNRR.

Purpose of the Study:

• To develop a novel biomimetic electrocatalyst for efficient eNRR.
• To investigate the structure-activity relationship of the proposed catalyst for enhanced ammonia synthesis.

Main Methods:

• Design and synthesis of a biomimetic elastic Mo single-atom protrusion on vanadium oxide support (pSA Mo/VOH).
• In situ spectroscopy and theoretical calculations to elucidate reaction mechanisms.
• Electrochemical performance testing for ammonia yield rate and Faradaic efficiency.

Main Results:

• The pSA Mo/VOH catalyst features a symmetry-breaking Mo site and an elastic Mo-O₄ pyramid.
• Optimized d-electron filling and enhanced N≡N bond polarization were observed.
• Achieved an excellent NH₃ yield rate of 50.71±1.12 μg h^-1 mg^-1 and a Faradaic efficiency of 35.38±1.03%.

Conclusions:

• The biomimetic elastic structure effectively optimizes the catalyst's electronic properties for eNRR.
• The dynamic Mo-O microenvironment facilitates efficient adsorption and hydrogenation of nitrogen intermediates.
• The developed electrocatalyst significantly outperforms existing catalysts for sustainable ammonia generation.