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N-H Bond Formation at a Diiron Bridging Nitride.
Angewandte Chemie International Edition ( IF 12.257 ) Pub Date : 2020-05-22 , DOI: 10.1002/anie.202006391
Shaoguang Zhang,Peng Cui,Tianchang Liu,Qiuran Wang,Thomas J Longo,Laura M Thierer,Brian C Manor,Michael R Gau,Patrick J Carroll,Georgia C Papaefthymiou,Neil Tomson

Despite their connection to ammonia synthesis, little is known about the ability of iron-bound, bridging nitrides to form N-H bonds. Herein we report a linear diiron bridging nitride complex supported by a redox-active macrocycle. The unique ability of the ligand scaffold to adapt to the geometric preference of the bridging species was found to facilitate the formation of N-H bonds via proton-coupled electron transfer to generate a µ-amide product. The structurally analogous µ-silyl- and µ-borylamide complexes were shown to form from the net insertion of the nitride into the E-H bonds (E = B, Si). Protonation of the parent bridging amide produced ammonia in high yield, and treatment of the nitride with PhSH was found to liberate NH3 in high yield through a reaction that engages the redox-activity of the ligand during PCET.
更新日期:2020-05-22

 

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