Bimetallic MOFs‐Derived NiFe2O4/Fe2O3 Enabled Dendrite‐free Lithium Metal Anodes with Ultra‐High Area Capacity Based on An Intermittent Lithium Deposition Model

Abstract 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.