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

As a promising alternative to the energy-intensive Haber–Bosch process, the electrochemical nitrogen reduction reaction (NRR) still faces challenges in catalyst development. This work demonstrates that vanadium doping is an effective strategy for significantly enhancing the NRR performance of MoSe2. A series of V-doped MoSe2 catalysts were synthesized via a one-step hydrothermal method. Comprehensive characterization reveals that moderate V doping multidimensionally modifies the electronic and architectural structure of MoSe2, and balancing of their variation can realize a promising enhancement of performance. The optimized catalyst (MSV-2, 4.92 atom % of V doping) achieves a superior ammonia yield rate of 28.37 μg h–1 mg–1 at −0.7 V and a higher Faradaic efficiency, far exceeding the performance of pristine MoSe2. Theoretical and experimental evidence demonstrates that the enhancement is attributed to the V incorporation-induced boost of N2 activation, facilitation of charge transfer, and effective suppression of the competing hydrogen evolution reaction. This study provides a fundamental understanding of the doping-induced optimization mechanism and offers a viable approach for designing high-performance, noble-metal-free electrocatalysts for sustainable ammonia synthesis.