Abstract
The first series of bis(silylene)‐stabilized nitrogen(I) compounds is described. Starting from the 1,2‐bis(N‐heterocyclic silylenyl) 1,2‐dicarba‐closo‐dedocaborane(12) scaffold 1, [1,2‐(LSi)2C2B10H10; L=PhC(NtBu)2], reaction with adamantyl azide (AdN3) affords the terminal N‐μ2‐bridged zwitterionic carborane‐1,2‐bis(silylium) AdN3 adduct 2 with an open‐cage dianionic nido‐C2B10 cluster core. Remarkably, upon one‐electron reduction of 2 with C8K and liberation of N2 and adamantane, the two silylene subunits are regenerated to furnish the isolable bis(silylene)‐stabilized NI complex as an anion of 3 with the nido‐C2B10 cluster cage. On the other hand, one‐electron oxidation of 2 with silver(I) yields the monocationic bis(silylene) NI complex 4 with the closo‐C2B10 cluster core. Moreover, the corresponding neutral NI radical complex 5 results from single‐electron transfer from 3 to 4.
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