The calculaOons suggest that the E d--Zn d+ is polarised with charge distribuOon shiied toward the central main group atom of 2a-c. Further comparisons with Cp*ZnZnCp*, Int-1, and TS-1 reveals that charge flow occurs from the breaking Zn-Zn bond to the main group centre with the Zn atoms becoming increasingly posiOve as the reacOon progresses (Figure ). These findings contradict the defining features of an oxidaOve process, i.e. that charge flow occurs from the site undergoing oxidaOve addiOon to the incoming substrate. At best the reacOon could be considered redox neutral and in the more extreme as a "reducOve addiOon" of Cp*ZnZnCp* to the main group carbene analogue. This hypothesis is further borne out by reacOvity. AddiOon of methyl iodide (MeI) to 2a over 16 h at 60 ° resulted in the formaOon of the corresponding dimethyl aluminium compound 1a-Me2 and Cp*ZnI, as major reacOon products. While small amounts of Cp*ZnMe were also observed in this reacOon, the implicaOon is that 2a is nucleophilic at aluminium consistent with charge localisaOon on this site.