Oxidation of [Li(THF)]2[Co(N=C(t)Bu2)4] with 1 equiv. of I2 generates Co(N=C(t)Bu2)4 in 85% yield. In the solid-state, this complex exhibits a squashed tetrahedral structure about the Co center. DFT calculations reveal this geometry arises, in part, to maximize ketimide-to-cobalt π-donation.

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Robust multivalent ion interaction in electrodes is a grand challenge of next-generation battery research. In this manuscript, we design molecularly-precise nanographene cathodes that are coupled with metallic Zn anodes to create a new class of Zn-ion batteries. Our results indicate that while electrodes with graphite or flat nanographenes do not support Zn-ion intercalation, the larger intermolecular spacing in a twisted peropyrene enables peropyrene electrodes to facilitate reversible Zn-ion intercalation in an acetonitrile electrolyte. While most previous Zn-ion batteries utilize aqueous electrolytes, the finding that nonaqueous Zn electrolytes can support intercalation in nanographenes is important for expanding the design space of nonaqueous multivalent batteries, which often possess higher voltages than their aqueous counterparts. Furthermore, because these nanographenes can be synthesized using a bottom-up approach via alkyne benzannulation, this work paves the way for future battery electrodes that contain other molecularly-precise nanographenes with tailored electrochemical properties.