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A radical anion based functionalization of the basal plane of two-dimensional(2D) materials is proposed in the present study. Simple charge neutral radicalfunctionalizations typically detach from the basal planes upon reduction. Forexample, epoxy oxygens irreversibly detach from graphene when reduced by analkali metal. The radical anion functionalization of 2D materials results in astable reduced state that can reversibly be oxidized and has high ionicconductivity due to the great mobility of the cations between the negativelycharged functional groups on the surface. Depending on the oxidation state ofthese systems, a high concentration of hole states can also be realizedallowing for good electronic conductivity. These properties can further allowfor improved energy storage devices via transition metal free cathode activespecies, solid electrolytes, electroconductive additives, separators, coatingsfor metal anodes and heat conductors through a single material. One possiblerealization of the above principles is the 2D salt An(BN)2OBX3, where A is analkali atom (Li, Na, etc; 0=<n=<2) or alkaline earth (Mg, etc; 0=<n=<1) and Xis a halide (typically F or Cl). This material can be derived from the basalplane functionalization of hexagonal boron nitride, h-BN, with .OBX3^- radicalanions in the presence of the A cations. One potential source of .OBX3^-radical anions is their recombined form, the [X3B-O-O-BX3]2- anion, which canbe found in the Lewis adduct of an AnO2 ionic peroxide with BX3:An[X3B-O-O-BX3]. The individual radical anions can be obtained by thermallysplitting the O-O bond in the recombined anion. Transition metal freeall-solid-state batteries with Li, Na and Mg anodes, thermal stability and highenergy and power densities may be realizable using An(BN)2OBX3.

Radical Anion Functionalization of Two-Dimensional Materials as a Means of Engineering Simultaneously High Electronic and Ionic Conductivity Solids