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Whereas the reduction of N-heterocyclic carbene (NHC)-stabilised cymantrenyldibromoboranes, (NHC)BBr\(_2\)Cym, in benzene results in formation of the corresponding diborenes (NHC)\(_2\)B\(_2\)Cym\(_2\), a change of solvent to THF yields a borylene of the form (NHC)\(_2\)BCym, stabilised through its boratafulvene resonance form.
In this contribution, we illustrate uranium complexes bearing a pendant borate (i.e. 1 and 2) or a pendant borane (i.e. 3 and 4) moiety via reaction of the highly strained uranacycle I with various 3‐coordinate boranes. Complexes 3 and 4 represent the first examples of uranium complexes with a pendant borane Lewis acid. Moreover, complex 3 was capable of activation of CO, delivering a new CO activation mode, and an abnormal CO 1,2‐insertion pathway into a U−N bond. The importance of the pendant borane moiety was confirmed by the controlled experiments.