Lithiation MXene Derivative Skeletons for Wide‐Temperature Lithium Metal Anodes

Lithium (Li) metal, as an appealing candidate for the next‐generation of high‐energy‐density batteries, is plagued by its safety issue mainly caused by uncontrolled dendrite growth and infinite volume expansion. Developing new materials that can improve the performance of Li‐metal anode is one of the urgent tasks. Herein, a new MXene derivative containing pure rutile TiO2 and N‐doped carbon prepared by heat‐treating MXene under a mixing gas, exhibiting high chemical activity in molten Li, is reported. The lithiation MXene derivative with a hybrid of LiTiO2‐Li3N‐C and Li offers outstanding electrochemical properties. The symmetrical cell assembling lithiation MXene derivative hybrid anode exhibits an ultra‐long cycle lifespan of 2000 h with an overpotential of ≈30 mV at 1 mA cm−2, which overwhelms Li‐based anodes reported so far. Additionally, long‐term operations of 34, 350, and 500 h at 10 mA cm−2 can be achieved in symmetrical cells at temperatures of −10, 25, and 50 °C, respectively. Both experimental tests and density functional theory calculations confirm that the LiTiO2‐Li3N‐C skeleton serves as a promising host for Li infusion by alleviating volume variation. Simultaneously, the superlithiophilic interphase of Li3N guides Li deposition along the LiTiO2‐Li3N‐C skeleton to avoid dendrite growth. A novel 3D LiTiO2‐Li3N‐C hybrid anode is first prepared by reacting molten Li with a MXene derivative, which exhibits outstanding electrochemical properties in a wide temperature range of ≈−10–50 °C by effectively prohibiting Li dendrite growth and volume fluctuation, dependent on a stable skeleton structure in combination with a superlithiophilic interphase of Li3N.