Dynamic Interphase-mediated Assembly for Deep Cycling Metal Batteries

Secondary batteries based on earth-abundant, multivalent metals provide a promising path for high energy density and potentially low-cost electricity storage. Poor anodic reversibility caused by disordered metal crystallization during battery charging remains a fundamental, century-old challenge for the practical use of deep cycling metal batteries. We report that dynamic interphases formed by anisotropic nanostructures dispersed in a battery electrolyte provide a general method for achieving ordered assembly of metal electrodeposits and high anode reversibility. Interphases formed by anisotropic graphitic carbon nitride nanostructures in colloidal electrolytes are shown to promote formation of vertically aligned and spatially compact (~100% compactness) zinc electrodeposits with unprecedented, high levels of reversibility (>99.8%), even at quite high areal capacity (6 to 20 milliampere hour per square centimeter). It is also reported that the same concept enables uniform growth of compact magnesium and aluminum electrodeposits, defining a general pathway toward energy-dense metal batteries based on earth-abundant anode chemistries.