The tight ion pair [EtZn (η3-C6H6)][CHB11Cl11]· C6H6 (1· C6H6) was obtained through β- hydrogen abstraction and concomitant ethene elimination from Et2Zn with the trityl salt [Ph3C][CHB11Cl11]. This ionlike species shows catalytic activity in hydrosilylation and intramolecular hydroamination reactions. The amine adduct {CH2CHCH2C (Ph2) CH2NH2} 3ZnCB11Cl11 (3), which features a rare transition metal− carborane σ bond, was isolated ...