Bimetallic MOFs-Derived NiFe 2 O 4 /Fe 2 O 3 Enabled Dendrite-free Lithium Metal Anodes with Ultra-High Area Capacity Based on An Intermittent Lithium Deposition Model.

In practical operating conditions, the lithium deposition behavior is often influenced by multiple coupled factors and there is also a lack of comprehensive and long-term validation for dendrite suppression strategies. Our group previously proposed an intermittent lithiophilic model for high-performance three-dimensional (3D) composite lithium metal anode (LMA), however, the electrodeposition behavior was not discussed. To verify this model, this paper presents a modified 3D carbon cloth (CC) backbone by incorporating NiFe 2 O 4 /Fe 2 O 3 (NFFO) nanoparticles derived from bimetallic NiFe-MOFs. Enhanced Li adsorption capacity and lithiophilic modulation were achieved by bimetallic MOFs-derivatives which prompted faster and more homogeneous Li deposition. The intermittent model was further verified in conjunction with the density functional theory (DFT) calculations and electrodeposition behaviors. As a result, the obtained Li-CC@NFFO||Li-CC@NFFO symmetric batteries exhibit prolonged lifespan and low hysteresis voltage even under ultra-high current and capacity conditions (5 mA cm -2 , 10 mAh cm -2 ), what's more, the full battery coupled with a high mass loading (9 mg cm -2 ) of LiFePO 4 cathode can be cycled at a high rate of 5 C, the capacity retention is up to 95.2 % before 700 cycles. This work is of great significance to understand the evolution of lithium dendrites on the 3D intermittent lithiophilic frameworks.