3D-Printed Electrodes for Lithium Metal Batteries with High Areal Capacity and High-Rate Capability

Abstract Lithium metal is the ultimate solution for high-energy density batteries, but is currently plagued from commercialization by the safety issue due to the uncontrollable Li dendrite growth. It would be worse when plating a higher areal capacity of lithium operating under higher current densities. Herein, we develop a novel N-doped carbon framework by extrusion-based 3D-printing of Zn-MOF precursor, which possess a hierarchically porous structure and a large specific surface area. Such unique structural features simultaneously suppress the dendrite growth, accommodate massive Li deposition, stabilize Li/electrolyte interface, and dissipate high current densities. As a result, the 3D-printed N-doped carbon framework (3DP-NC) enables an ultrahigh areal capacity of 30 mAh cm-2 at the high rate of 10 mA cm-2 and a high average Coulombic efficiency of 97.9% after a long lifespan of ∼2000 h at the rate of 1 mA cm-2. Moreover, the Li-plated 3DP-NC anode is capable of working properly under an ultrahigh rate of 20 mA cm-2 in symmetric cells with low overpotentials and manifesting a much-enhanced rate capability in full cells with a 3D-printed LiFePO4 cathode. The 3D-printing strategy demonstrated in the present work provides a promising new avenue for the fabrication of high-performance Li-metal batteries.