High-Energy Symmetric Li-Ion Battery Enabled by Binder-Free FeOF-MXene Heterostructure with Doubly Matched Capacity and Kinetics

Fluorides are viewed as promising conversion-type Li-ion battery cathodes to meet the desired high energy density. FeOF is a typical member of conversion-type fluorides, but its major drawback is sluggish kinetics upon deep discharge. Herein, a heterostructured FeOF-MXene composite (FeOF-MX) is demonstrated to overcome this limitation. The rationally designed FeOF-MX electrode features a microsphere morphology consisting of closely packed FeOF nanoparticles, providing fast transport pathways for lithium ions while a continuous wrapping network of MXene nanosheets ensures unobstructed electron transport, thus enabling high-rate lithium storage with enhanced pseudocapacitive contribution. In/ex situ characterization techniques and theoretical calculations, both reveal that the lithium storage mechanism in FeOF arises from a hybrid intercalation-conversion process, and strong interfacial interactions between FeOF and MXene promote Li-ion adsorption and migration. Remarkably, through demarcating the conversion-type reaction with a controlled potential window, a symmetric full battery with prelithiated FeOF-MX as both cathode and anode is fabricated, achieving a high energy density of 185.5 Wh kg-1 and impressive capacity retention of 88.9% after 3000 cycles at 1 A g-1. This work showcases an effective route toward high-performance MXene engineered fluoride-based electrodes and provides new insights into constructing symmetric batteries yet with high-energy/power densities. An electrostatic self-asembly strategy is proposed to synthesize FeOF-MXene heterostructure, in which Li+ charge storage in FeOF arises from an intercalation-conversion hybrid reactions process, and strong interfacial interactions between FeOF and MXene promote Li-ion adsorption and migration. The as-built symmetric battery based on FeOF-MXene heterostructure with matchable capacity and kinetics achieves a high energy of 185.5 Wh kg-1. image