Multidimensional Manipulation of MoSe₂ Enabled by Vanadium Doping for Efficient Nitrogen Reduction.

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• The Haber-Bosch process for ammonia synthesis is energy-intensive.
• Electrochemical nitrogen reduction reaction (NRR) is a promising alternative but faces catalyst challenges.
• Developing efficient, noble-metal-free catalysts is crucial for sustainable ammonia production.

Purpose of the Study:

• To investigate vanadium (V) doping as a strategy to enhance the NRR performance of molybdenum diselenide (MoSe2).
• To understand the mechanism by which V doping optimizes MoSe2 for NRR.
• To develop a high-performance, noble-metal-free electrocatalyst for sustainable ammonia synthesis.

Main Methods:

• Synthesis of V-doped MoSe2 catalysts using a one-step hydrothermal method.
• Comprehensive characterization of catalyst structure and electronic properties.
• Electrochemical evaluation of NRR performance, including ammonia yield rate and Faradaic efficiency.
• Theoretical and experimental analysis of doping-induced mechanisms.

Main Results:

• Moderate V doping multidimensionally modifies the electronic and architectural structure of MoSe2.
• The optimized catalyst (MSV-2, 4.92 atom % V) achieved an ammonia yield rate of 28.37 μg h⁻¹ mg⁻¹ at -0.7 V with high Faradaic efficiency.
• V incorporation boosted N2 activation, facilitated charge transfer, and suppressed the hydrogen evolution reaction.
• Performance significantly exceeded that of pristine MoSe2.

Conclusions:

• Vanadium doping is an effective strategy for enhancing MoSe2-based NRR electrocatalysts.
• Optimized V doping balances structural and electronic modifications for superior performance.
• This work provides fundamental insights into doping mechanisms for catalyst design and offers a viable approach for sustainable ammonia synthesis.