Ammonia Formation Catalyzed by a Dinitrogen-Bridged Dirhenium Complex Bearing PNP-Pincer Ligands under Mild Reaction Conditions**

Fanqiang Meng, Shogo Kuriyama, Hiromasa Tanaka, Akihito Egi, Kazunari Yoshizawa, Yoshiaki Nishibayashi

Research output: Contribution to journalArticlepeer-review

Abstract

A series of rhenium complexes bearing a pyridine-based PNP-type pincer ligand are synthesized from rhenium phosphine complexes as precursors. A dinitrogen-bridged dirhenium complex bearing the PNP-type pincer ligands catalytically converts dinitrogen into ammonia during the reaction with KC8 as a reductant and [HPCy3]BArF4 (Cy=cyclohexyl, ArF=3,5-(CF3)2C6H3) as a proton source at −78 °C to afford 8.4 equiv of ammonia based on the rhenium atom of the catalyst. The rhenium-dinitrogen complex also catalyzes silylation of dinitrogen in the reaction with KC8 as a reductant and Me3SiCl as a silylating reagent under ambient reaction conditions to afford 11.7 equiv of tris(trimethylsilyl)amine based on the rhenium atom of the catalyst. These results demonstrate the first successful example of catalytic nitrogen fixation under mild reaction conditions using rhenium-dinitrogen complexes as catalysts.

Original languageEnglish
Pages (from-to)13906-13912
Number of pages7
JournalAngewandte Chemie - International Edition
Volume60
Issue number25
DOIs
Publication statusPublished - Jun 14 2021

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

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