). With the successful synthesis of the chiral cobaltacycle intermediates, the stoichiometric reactions of intermediates 45 and 46 with allene 2 provided the desired product 3 (52% yield) and 31 (41% yield) with high enantiocontrol supporting a Co(III/I/II) pathway (Scheme 5C). Furthermore, we probed the enantioselective electrochemical C-H annulation by means of voltammetric analysis (Scheme 5D). While cobalt acetate with NaOPiv showed no relevant redox behavior in the solvent system of catalysis, the addition of ligand L3 leads to clear oxidation events in the cyclic voltammogram. The waves are attributable to cobalt species mono-and biscoordinated by ligand L3. At 0.8 V (vs SCE) a reversible wave is visible when L3 is combined with cobalt acetate, whereby it is noticeable that the reversibility is significantly less pronounced with the addition of substrate 1 further supporting the Co(III/I/II) pathway (Figure S-1 and S-2 in the Supporting Information).