Regulating Ion Transport in Lithium Metal Batteries via Metal‐Organic Frameworks Electrolyte Modulator

Abstract Low Li + transference number in liquid electrolytes can lead to uneven lithium deposition and dendrite growth, reducing coulombic efficiency and cycle life of lithium metal batteries. In this study, metal‐organic frameworks (MOFs) are used as electrolyte modulator to regulate Li + transport. The ‐NH 2 group introduced into MOFs can form hydrogen bonds with anions in the electrolyte, immobilizing these anions and thereby facilitating the migration of cations. As a result, a uniform and dense deposition morphology of lithium was achieved. The Li + transference number is increased from 0.26 to 0.57. The assembled Li||Li symmetrical cell can stably cycle for over for 900 h with an average overpotential below 20 mV. In addition, the rate performance of the battery can be enhanced.