Single‐Atom Lithiophilic Sites Confined within Ordered Porous Carbon for Ultrastable Lithium Metal Anodes

Abstract

Attributing to the high specific capacity and low electrochemical reduction potential, lithium (Li) metal is regarded as the most promising anode for high‐energy Li batteries. However, the growth of lithium dendrites and huge volume change seriously limit the development of lithium metal batteries. To overcome these challenges, an ordered mesoporous N‐doped carbon with lithiophilic single atoms is proposed to induce uniform nucleation and deposition of Li metal. Benefiting from the synergistic effects of interconnected three‐dimensional ordered mesoporous structures and abundant lithiophilic single‐atom sites, regulated local current density and rapid mass transfer can be achieved, leading to the uniform Li deposition with inhibition of dendrites and buffered volume expansion. As a result, the as‐fabricated anode exhibits a high CE of 99.8% for 200 cycles. A stable voltage hysteresis of 14 mV at 5 mA cm−2 could be maintained for more than 1330 h in the symmetric cell. Furthermore, the full cell coupled with commercial LiFePO4 exhibits high reversible capacity of 108 mAh g−1 and average Coulombic efficiency of 99.8% from 5th to 350th cycles at 1 C. The ordered mesoporous carbon host with abundant lithiophilic single‐atom sites delivers new inspirations into rational design of high‐performance Li metal anodes.