Issue 15, 2025

Computational screening aided design of single atom-doped MoS2 as electrocatalysts in nitrogen fixation

Abstract

Nitrogenase's structure has catalyzed the evolution of bio-inspired catalysts, specifically transition metal sulfides, echoing the enzyme's cofactor architecture. Molybdenum-based derivatives, mirroring nitrogenase's active sites, demonstrate potential in electrochemical nitrogen reduction for ambient ammonia synthesis. However, achieving an optimal balance between nitrogen activation and hydrogen production presents a significant hurdle. To address this, we utilized MoS2, structurally akin to natural nitrogenase, decorated with doped transition single atoms to enhance catalytic performance. Employing accelerated high-throughput density functional theory (DFT) calculations, W-doped MoS2 with sulfur vacancies (Sv-W-MoS2) was identified as a leading candidate, showcasing improved selectivity for N2 activation while maintaining a hydrogen production profile akin to nitrogenase's NH3 synthesis, often accompanied by a proportionate amount of H2. Experimental validation confirmed the superior NH3 generation capacity of Sv-W-MoS2, achieving a substantial yield of 62.42 μg h−1 cm−2 with a faradaic efficiency of 22.34% under alkaline conditions at −0.5 V versus the reversible hydrogen electrode (vs. RHE), outshining other metal-doped MoS2 variants. This breakthrough offers a solid theoretical framework for the development of bio-inspired nitrogen reduction reaction (NRR) catalysts, aiming to harmonize nitrogen activation with hydrogen production.

Graphical abstract: Computational screening aided design of single atom-doped MoS2 as electrocatalysts in nitrogen fixation

Supplementary files

Article information

Article type
Paper
Submitted
09 Dec 2024
Accepted
06 Mar 2025
First published
07 Mar 2025

J. Mater. Chem. A, 2025,13, 10666-10674

Computational screening aided design of single atom-doped MoS2 as electrocatalysts in nitrogen fixation

G. Hai, G. Chen, K. Gong and X. Huang, J. Mater. Chem. A, 2025, 13, 10666 DOI: 10.1039/D4TA08748H

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