N–N Bond Cleavage of Mid-Valent Ta(IV) Hydrazido
and Hydrazidium Complexes Relevant to the Schrock Cycle for Dinitrogen
Fixation
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Abstract
Chemical
reduction of the Ta(V) hydrazido chloride <b>1</b> generates
the open-shell, mononuclear Ta(IV) hydrazido complex <b>2</b>, which upon N-methylation yields the corresponding structurally
characterized Ta(IV) hydrazidium <b>6</b>. Chemical reduction
of <b>6</b> results in N–N bond cleavage to generate
a cis/trans mixture of the [Ta(V),Ta(V)] bis(μ-nitrido) product <b>7</b> in tetrahydrofuran and the mononuclear Ta(V) parent imide <b>8</b> in toluene. These results serve to establish an important
foundation for the pursuit of a group-5 metal variant of the Schrock
cycle for dinitrogen fixation