Abstract
A series of group 11 metal complexes coordinated by (nitronyl nitroxide)‐2‐ide radical anion NN‐M(dtpb) [NN: nitronyl nitroxide; M: CuI, AgI, and AuI; dtpb: 1,2‐bis(di‐2‐tolylphosphanyl)benzene)] was prepared. Their structures, electrochemical properties, and related theoretical calculations were investigated. The oxidation potential (Eox, V vs. Fc/Fc+) of the NN‐moiety in these radical‐metalloids significantly shifted to the negative direction in comparison to that of the unsubstituted nitronyl nitroxide (NN‐H, Eox = +0.38 V); this is strongly dependant on the metal ion (Eox = –0.37 V for M = CuI, –0.31 V for AgI, and –0.28 V for AuI). The Eox values correlated with the energy level of the HOMO (SOMO) and also with the natural atomic charge of the C2 carbon atom attached to the metal ion, indicating that the ionic character of the metal–C2–carbon bond is a key factor in controlling the oxidation potential of these radical metalloids.
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