Unraveling N–O Cleavage and N–H Bond Formation for NO Reduction to NH <sub>3</sub> at a Bimetallic Fe–Mo Site

Reductive transformation of nitric oxide (NO) by heme proteins is critical for dissimilatory nitrate reduction to ammonium, a microbial nitrogen-conserving process. This study reports the complete reduction of bound NO to NH 3 on a bimetallic FeMo platform through a protonation-hydride reduction strategy. Protonation of the μ-NO group generated a μ-NOH intermediate, which, upon reaction with HBpin, underwent simultaneous N–O bond cleavage and N–H bond formation to give a μ-NH imide. Subsequent transformations among nitride, imide, and amide were achieved via deprotonation/protonation and the additions of hydride, hydrogen atoms, and H 2 provide molecular-level mechanistic insight into ammonia synthesis and nitrogenous-species interconversion.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2026-06-18
DOI
https://doi.org/10.1021/jacs.6c01633
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
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article

Unraveling N–O Cleavage and N–H Bond Formation for NO Reduction to NH 3 at a Bimetallic Fe–Mo Site

Shengfa Ye, Rong‐Zhen Liao, Xiaofang Zhai, Chen‐Ho Tung et al.
Journal of the American Chemical Society
Ammonia Synthesis and Nitrogen Reduction
article

Unraveling N–O Cleavage and N–H Bond Formation for NO Reduction to NH 3 at a Bimetallic Fe–Mo Site

Shengfa Ye, Rong‐Zhen Liao, Xiaofang Zhai, Chen‐Ho Tung, Li‐Zhu Wu, Tianyi Geng, Wenguang Wang, Xuebin Jiang, Y H Wu
article en

Abstract

Reductive transformation of nitric oxide (NO) by heme proteins is critical for dissimilatory nitrate reduction to ammonium, a microbial nitrogen-conserving process. This study reports the complete reduction of bound NO to NH 3 on a bimetallic FeMo platform through a protonation-hydride reduction strategy. Protonation of the μ-NO group generated a μ-NOH intermediate, which, upon reaction with HBpin, underwent simultaneous N–O bond cleavage and N–H bond formation to give a μ-NH imide. Subsequent transformations among nitride, imide, and amide were achieved via deprotonation/protonation and the additions of hydride, hydrogen atoms, and H 2 provide molecular-level mechanistic insight into ammonia synthesis and nitrogenous-species interconversion.

Journal of the American Chemical Society
Ministry of Education of the People's Republic of China (CN), Sun Yat-sen University (CN), Dalian Institute of Chemical Physics (CN), Chinese Academy of Sciences (CN), Beijing Normal University (CN), Institute of Catalysis and Petrochemistry (RU), Second Hospital of Shandong University (CN), Technical Institute of Physics and Chemistry (CN), Qilu Hospital of Shandong University (CN), University of Chinese Academy of Sciences (CN), State Key Laboratory of Catalysis, Huazhong University of Science and Technology (CN)
Openalex Percentile: Top 19%
Ammonia Synthesis and Nitrogen Reduction
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