Radical anion functionalization of two-dimensional materials as a means of engineering simultaneously high electronic and ionic conductivity solids.

摘要: A radical anion based functionalization of the basal plane hexagonal boron nitride (h-BN) and other two-dimensional (2D) materials is proposed in present study. The resulting can reversibly be oxidized without detachment functional groups from thus serve as surface-intercalation type cathode electroactive species fast solid ion conductors at same time. h-BN with [·OBX3]-radical anions (X=F,Cl) presence Li, Na or Mg cations provides one example such systems. This material realized a simple, two step synthesis. In first step, symmetric Lewis adduct corresponding peroxides formed BX3. second thermally split into identical that covalently functionalize B atoms h-BN. maximum density surface packing functionalization, product synthesis An[(BN)2OBX3] (A=Li,Na n=1 A=Mg n=0.5). highly states (0≤n≤1 for Li 0≤n≤0.5 Mg), electronic conductivity this order 1 S/cm, similar to carbon black. fully reduced (n=2 becomes an insulator, like tunability properties via cation concentration allows its application multifunctional energy storage devices, simultaneously serving active species, electrolyte, electroconductive additive, separator, heat conductor coating metal anodes enables dendrite-free plating. multifunctionality reduces number phases needed all-solid-state battery supercapacitor interfacial impedance making devices more efficient. For example, Li[(BN)2OBF3] predicted have 5.6 V open circuit voltage vs anode, capacity 191 mAh/g, specific 1067 Wh/kg store (materials only) cost 24 USD/kWh.