Potent anionophilic bimetallic frameworks enabling lithium dendrite-free deposition for high-performance lithium batteries

Lithium metal batteries (LMBs) have attracted significant attention due to their high theoretical capacity and low electrochemical potential. However, the growth of lithium dendrites severely restricts their practical applications. In this study, a zeolite imidazolate-based nano-BMOF (ZNB) electrolyte additive is proposed to effectively inhibit the growth of lithium dendrites by regulating the anion distribution and promoting the uniform deposition of lithium ions. The experimental results demonstrate that the ZNB-modified electrolyte significantly improves the electrochemical performance and achieves dendrite-free lithium deposition on copper electrodes. The strong anion adsorption by ZNB and its role in promoting lithium-ion solvation were further verified using density-functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations. In Li||NCM523 batteries, the ZNB electrolyte achieves a capacity retention rate of 91 % after 200 cycles and a Coulombic efficiency of 99.03 %. In addition, the ZNB electrolyte significantly reduces the battery overpotential and improves the transport kinetics of lithium ions. This study presents a new approach to inhibit lithium dendrite growth and enhance the electrochemical performance of lithium metal batteries.