Vertically Aligned Conductive Metal–Organic Frameworks with Switchable Electrical Conductivity for Li Metal Anode

Abstract Lithium (Li) metal, with its unparalleled theoretical capacity and lowest electrochemical potential, is a promising anode material for rechargeable batteries. Yet, challenges such as dendrite formation, severe electrode volume change, and ongoing Li consumption impede its practical adoption. To address these challenges, a novel approach is introduced, harnessing the switchable electrical conductivity of a nanoporous current collector for Li metal anode. A vertically aligned Nickel‐catecholate (VANC) is directly grown on the copper foil as the nanoporous current collector, and the Li intercalation and de‐intercalation of VANC reversibly decrease and increase the electrical conductivity in the direction perpendicular to the electrode, respectively. The switchable conductivity induces uniform deposition and stripping of Li metal without forming dendrite and dead Li during the Li plating/stripping process and thus enables high coulombic efficiency of over 98% even after 200 cycles. This nanoporous structure with switchable conductivity will open up a new path for reliable lithium metal anode for rechargeable battery applications.