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N-H Bond Formation at a Diiron Bridging Nitride.
Zhang, Shaoguang; Cui, Peng; Liu, Tianchang; Wang, Qiuran; Longo, Thomas J; Thierer, Laura M; Manor, Brian C; Gau, Michael R; Carroll, Patrick J; Papaefthymiou, Georgia C; Tomson, Neil C.
Afiliación
  • Zhang S; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Cui P; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Liu T; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Wang Q; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Longo TJ; Department of Physics, Villanova University, Villanova, PA, 19085, USA.
  • Thierer LM; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Manor BC; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Gau MR; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Carroll PJ; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
  • Papaefthymiou GC; Department of Physics, Villanova University, Villanova, PA, 19085, USA.
  • Tomson NC; P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104, USA.
Angew Chem Int Ed Engl ; 59(35): 15215-15219, 2020 08 24.
Article en En | MEDLINE | ID: mdl-32441448
ABSTRACT
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.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Transporte de Electrón / Nitrógeno Idioma: En Revista: Angew Chem Int Ed Engl Año: 2020 Tipo del documento: Article País de afiliación: Estados Unidos
Texto completo
Añadir a Mi BVS
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XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Transporte de Electrón / Nitrógeno Idioma: En Revista: Angew Chem Int Ed Engl Año: 2020 Tipo del documento: Article País de afiliación: Estados Unidos