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• W1967014760 endingPage "17098" @default.
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• W1967014760 abstract "Activation of molecular nitrogen by transition metal complexes is an area of current interest as investigations using the inert N 2 molecule to produce higher-value organonitrogen compounds intensify. In an attempt to extend the addition of hydride reagents E-H (where E = BR 2 , AlR 2 , and SiR 3 ) to the dinitrogen complex ([NPN]Ta) 2 (μ-H) 2 (μ-η 1 :η 2 -N 2 ) [1; where NPN = (PhNSiMe 2 CH 2 ) 2 PPh], the reaction with zirconocene chlorohydride, [Cp 2 Zr(Cl)H] x , was examined. The crystalline product formed in 35% yield was determined to be ([NP(N)N]Ta)(μ-H) 2 (μ-N)(Ta[NPN])(ZrCp 2 ) ( 2 ) in which the coordinated N 2 has been cleaved to form a phosphinimide bridging between Ta and Zr and a triply bridging nitride. The mechanism of this reaction was examined to determine the fate of the chloride and hydride ligands attached to Zr in the starting zirconocene reagent. Using the zirconocene dihydride dimer ([Cp 2 ZrH 2 ] 2 ), a higher yield of 2 was obtained (76%), and H 2 was also observed by 1 H NMR spectroscopy. To probe the origin of the eliminated H 2 , the dideuterated dinitrogen complex ([NPN]Ta) 2 (μ-D) 2 (μ-η 1 :η 2 -N 2 ) ( d 2 -1) was allowed to react with ([Cp 2 ZrH 2 ] 2 ), which resulted in the formation of ([NP(N)N]Ta)(μ-D) 2 (μ-N)(Ta[NPN])(ZrCp 2 ), ( d 2 -2), with no evidence of hydrogen for deuterium scrambling between the starting zirconocene dihydride and the ditantalum dinitrogen complex. Studies into the use of preformed Zr(II) and Ti(II) reagents were also performed. The proposed mechanism involves initial adduct formation that facilitates inner-sphere electron transfer to cleave the N-N bond to form a species with bridging nitrides, one of which is transformed by nucleophilic attack of a phosphine donor to generate the observed phosphinimide." @default.
• W1967014760 created "2016-06-24" @default.
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• W1967014760 date "2006-11-14" @default.
• W1967014760 modified "2023-09-25" @default.
• W1967014760 title "Inner-sphere two-electron reduction leads to cleavage and functionalization of coordinated dinitrogen" @default.
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• W1967014760 doi "https://doi.org/10.1073/pnas.0602132103" @default.
• W1967014760 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/1693869" @default.
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