Ultra‐Uniform and Functionalized Nano‐Ion Divider for Regulating Ion Distribution toward Dendrite‐Free Lithium‐Metal Batteries

Abstract Ionic dividers with uniform pores and functionalized surfaces display significant potential for solving Li‐dendrite issues in Li‐metal batteries. In this study, single metal and nitrogen co‐doped carbon‐sandwiched MXene (M‐NC@MXene) nanosheets are designed and fabricated, which possess highly ordered nanochannels with a diameter of ≈10 nm. The experiments and computational calculations verified that the M‐NC@MXene nanosheets eliminate Li dendrites in several ways: (1) redistributing the Li‐ion flux via the highly ordered ion channels, (2) selectively conducting Li ions and anchoring anions by heteroatom doping to extend the nucleation time for Li dendrites, and (3) tightly staggering on a routine polypropylene (PP) separator to obstruct the growth path of Li dendrites. With a Zn‐NC@MXene‐coated PP divider, the assembled Li||Li symmetric battery shows an ultralow overpotential of ≈25 mV and a cycle life of 1500 h at a high current density of 3 mA cm⁻² and high capacity of 3 mAh cm⁻². Remarkably, the life of a Li||Ni83 pouch cell with an energy density of 305 Wh kg⁻¹ is improved by fivefold. Moreover, the remarkable performance of Li||Li, Li||LiFePO₄, and Li||sulfur batteries reveal the significant potential of the well‐designed multifunctional ion divider for further practical applications.