Designing V Single Atom Embedded Carbon Moiety for the Electrocatalytic Nitrogen Reduction Reaction by First...

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• The Haber-Bosch process, while vital for ammonia production, is energy-intensive.
• Developing efficient electrocatalysts for the nitrogen reduction reaction (NRR) offers a sustainable alternative.
• Single-atom catalysts (SACs) are promising due to their high atom utilization efficiency.

Purpose of the Study:

• To investigate vanadium-based single-atom catalysts (SACs) for NRR activity.
• To explore how varying the coordination environment of vanadium atoms impacts catalytic performance.
• To identify promising SACs as alternatives to the Haber-Bosch process.

Main Methods:

• Density Functional Theory (DFT) calculations were employed to study vanadium SACs.
• Investigated phthalocyanine, porphyrin, and graphene-like coordination environments with varying nitrogen coordination.
• Examined the electrocatalytic properties of vanadium phthalocyanine (V_phN₄) on an Ag(111) surface.

Main Results:

• Vanadium phthalocyanine (V_phN₄) emerged as the most promising system.
• V_phN₄ demonstrated high selectivity for NRR over the hydrogen evolution reaction (HER).
• The system exhibited strong binding of N₂ relative to H, preventing hydrogen poisoning, and the lowest overpotential among studied systems.

Conclusions:

• Vanadium phthalocyanine (V_phN₄) is a highly promising single-atom catalyst for the nitrogen reduction reaction.
• The V_phN₄ monolayer on Ag(111) shows excellent potential for catalytic electrode applications.
• This research contributes to the development of sustainable ammonia synthesis methods.