1. Dinitrogen cleavage and hydrogenation to ammonia with a uranium complex.
- Author
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Xin, Xiaoqing, Douair, Iskander, Zhao, Yue, Wang, Shuao, Maron, Laurent, and Zhu, Congqing
- Subjects
HABER-Bosch process ,HYDROGENATION ,AMMONIA ,URANIUM ,MANUFACTURING processes ,NITROGEN - Abstract
The Haber–Bosch process produces ammonia (NH
3 ) from dinitrogen (N2 ) and dihydrogen (H2 ), but requires high temperature and pressure. Before iron-based catalysts were exploited in the current industrial Haber–Bosch process, uranium-based materials served as effective catalysts for production of NH3 from N2 . Although some molecular uranium complexes are known to be capable of combining with N2 , further hydrogenation with H2 forming NH3 has not been reported to date. Here, we describe the first example of N2 cleavage and hydrogenation with H2 to NH3 with a molecular uranium complex. The N2 cleavage product contains three uranium centers that are bridged by three imido μ2 -NH ligands and one nitrido μ3 -N ligand. Labeling experiments with15 N demonstrate that the nitrido ligand in the product originates from N2 . Reaction of the N2 -cleaved complex with H2 or H+ forms NH3 under mild conditions. A synthetic cycle has been established by the reaction of the N2 -cleaved complex with trimethylsilyl chloride. The isolation of this trinuclear imido-nitrido product implies that a multi-metallic uranium assembly plays an important role in the activation of N2 . [ABSTRACT FROM AUTHOR]- Published
- 2023
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