Ultrahigh-capacity and dendrite-free lithium metal anodes enabled by lithiophilic bimetallic oxides

Abstract

The commercialization of lithium (Li) metal anodes is greatly hindered by dendritic Li growth, infinite volume change, “dead Li”, and a fragile solid electrolyte interphase. A series of bimetallic oxides, including ZnMn₂O₄, ZnCo₂O₄, and NiCo₂O₄ are developed as a new class of lithiophilic materials for stable Li metal anodes. Benefitting from the synergistic effect of different metal cations, the bimetallic oxide modified carbon cloths demonstrate impressive capabilities in suppressing dendritic Li growth at high areal capacities up to 20 mA h cm⁻². Compared with the monometallic oxide modified hosts, ZnMn₂O₄@CC exhibits a much longer lifespan up to 1900 h at a high current density/areal capacity of 10 mA cm⁻²/10 mA h cm⁻². When paired with LiFePO₄, the full cell could maintain a capacity retention capability of 89.4% after 350 cycles at 2 C. The bimetallic oxide-based lithiophilic materials can not only boost practical Li metal batteries, but also shed light on other lithiophilic classes such as bimetallic sulfides/selenides.