Ultrahigh-current density anodes with interconnected Li metal reservoir through overlithiation of mesoporous AlF₃...

Lithium (Li) metal is the ultimate solution for next-generation high-energy density batteries but is plagued from commercialization by infinite relative volume change, low Coulombic efficiency due to side reactions, and safety issues caused by dendrite growth. These hazardous issues are further aggravated under high current densities needed by the increasing demand for fast charging/discharging. We report a one-step fabricated Li/Al₄Li₉-LiF nanocomposite (LAFN) through an "overlithiation" process of a mesoporous AlF₃ framework, which can simultaneously mitigate the abovementioned problems. Reaction-produced Al₄Li₉-LiF nanoparticles serve as the ideal skeleton for Li metal infusion, helping to achieve a near-zero volume change during stripping/plating and suppressed dendrite growth. As a result, the LAFN electrode is capable of working properly under an ultrahigh current density of 20 mA cm^-2 in symmetric cells and manifests highly improved rate capability with increased Coulombic efficiency in full cells. The simple fabrication process and its remarkable electrochemical performances enable LAFN to be a promising anode candidate for next-generation lithium metal batteries.