期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 20, 页码 6674-6677出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201902195
关键词
ammonia; dinitrogen reduction; frustrated Lewis pairs; nitrogen fixation; titanium
资金
- UK EPSRC [EP/M027015/1, EP/P001286/1]
- ERC [CoG612724]
- Royal Society [UF110005]
- University of Manchester
- EPSRC [EP/P001386/1, EP/M027015/1] Funding Source: UKRI
- Royal Society [UF110005] Funding Source: Royal Society
Although reductive cleavage of dinitrogen (N-2) to nitride (N3-) and hydrogenation with dihydrogen (H-2) to yield ammonia (NH3) is accomplished in heterogeneous Haber-Bosch industrial processes on a vast scale, sequentially coupling these elementary reactions together with a single metal complex remains a major challenge for homogeneous molecular complexes. Herein, we report that the reaction of a chloro titanium triamidoamine complex with magnesium effects complete reductive cleavage of N-2 to give a dinitride dititanium dimagnesium ditriamidoamine complex. Tandem H-2 splitting by a phosphine-borane frustrated Lewis pair (FLP) shuttles Hatoms to the N3-, evolving NH3. Isotope labelling experiments confirmed N-2 and H-2 fixation. Though not yet catalytic, these results give unprecedented insight into coupling N-2 and H-2 cleavage and N-H bond formation steps together, highlight the importance of heterobimetallic cooperativity in N-2 activation, and establish FLPs in NH3 synthesis.
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