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• W1479896687 abstract "The ability of certain transition metals to mediate the reduction of N2 to NH3 has attracted broad interest in the biological and inorganic chemistry communities. Early transition metals such as Mo and W readily bind N2 and mediate its protonation at one or more N atoms to furnish M(NxHy) species that can be characterized and, in turn, extrude NH3. By contrast, the direct protonation of Fe–N2 species to Fe(NxHy) products that can be characterized has been elusive. Herein, we show that addition of acid at low temperature to [(TPB)Fe(N2)][Na(12-crown-4)] results in a new S = 1/2 Fe species. EPR, ENDOR, Mössbauer, and EXAFS analysis, coupled with a DFT study, unequivocally assign this new species as [(TPB)Fe≡N–NH2]+, a doubly protonated hydrazido(2−) complex featuring an Fe-to-N triple bond. This unstable species offers strong evidence that the first steps in Fe-mediated nitrogen reduction by [(TPB)Fe(N2)][Na(12-crown-4)] can proceed along a distal or “Chatt-type” pathway. A brief discussion of whether subsequent catalytic steps may involve early or late stage cleavage of the N–N bond, as would be found in limiting distal or alternating mechanisms, respectively, is also provided." @default.
• W1479896687 created "2016-06-24" @default.
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• W1479896687 date "2015-06-10" @default.
• W1479896687 modified "2023-10-11" @default.
• W1479896687 title "Characterization of an Fe≡N–NH₂ Intermediate Relevant to Catalytic N₂ Reduction to NH₃" @default.
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• W1479896687 doi "https://doi.org/10.1021/jacs.5b03432" @default.
• W1479896687 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/4603982" @default.
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