Sc-Doped Sulfur Vacancy MoS₂ Photocatalytic Nitrogen Reduction to Ammonia: Experimental and Theoretical Investigation.

Authors

Lianyang Zhang, Zhiling Huang, Shengjie Xia

Published in

Inorganic chemistry. Jul 18, 2025. Epub Jul 18, 2025.

Abstract

This paper combines defect engineering and metal doping to prepare transition metal Sc-doped molybdenum sulfide-containing sulfur vacancies (Sc@V_S-MoS₂), which is used for photocatalytic nitrogen reduction to synthesize ammonia (pNRR). The activity of Sc@V_S-MoS₂ for pNRR is as high as 124.26 μmol g^-1 h^-1, which is 6.16, 2.23, and 2.69 times for MoS₂, V_S-MoS₂, and Sc@MoS₂, respectively. This indicates that the combination of S vacancies and Sc doping can significantly improve the photocatalytic performance of MoS₂ materials. Theoretical calculations show that the energy barrier U_L of the potential determining step (PDS) is only -0.393 V, much lower than V_S-MoS₂, making Sc@V_S-MoS₂ exhibit excellent nitrogen reduction activity for ammonia synthesis. Computational results demonstrate that Sc@V_S-MoS₂ exhibits outstanding N₂ adsorption and activation properties, with 0.533 e charge transfer to N₂ that significantly reduces the free energy barrier for the first hydrogenation step. Moreover, its hydrogen adsorption free energy is substantially lower than that of V_S-MoS₂, effectively suppressing the competing hydrogen evolution reaction and enhancing N₂ reduction selectivity. In situ infrared spectroscopy showed the formation of -N₂H_y species on the catalyst surface, indicating that the enzyme pathway is the most likely reaction pathway, consistent with the calculated results.

PMID:
40680184
Bibliographic data and abstract were imported from PubMed on 19 Jul 2025.

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