Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti3C2Tx MXene Intermediate Layer

The propensity of Li to form irregular and nonplanar electrodeposits has become a fundamental barrier for fabricating Li metal batteries. Here, a planar, dendrite-free Li metal growth on 2D Ti 3 C 2 T x MXene is reported. Ab initio calculations suggest that Li forms a hexagonal close-packed ( hcp ) layer on the surface of Ti 3 C 2 T x via ionic bonding and the lattice confinement. The ionic bonding weakens gradually after a few monolayers, resulting in a nanometers-thin transition region of hcp -Li. Above this transition region, the deposition is dominated by plating of body-centered cubic ( bcc ) Li via metallic bonding. Formation of a dense and planar Li metal anode with preferential growth along the (110) facet is explained by the lattice matching between Ti 3 C 2 T x and hcp -Li and then with bcc -Li, as well as preferred thermodynamic factors including the large dendrite formation energy and small migration barrier for Li. The prepared Li metal anode shows stable cycling in a wide current density range from 0.5 to 10.0 mA cm –2 . The LiFePO 4 ‖Li full cell fabricated with this Li metal anode exhibits only 9.5% capacity fading after 500 charge–discharge cycles at 1 C rate.