Lithiophilic onion-like carbon spheres as lithium metal uniform deposition host

Lithium metal is considered as a promising anode material for next-generation secondary batteries, owing to its high theoretical specific capacity (3860 mA h g^-1). Nevertheless, the practical application of Li in lithium metal batteries (LMBs) is hampered by inhomogeneous Li deposition and irreversible "dead Li", which lead to low coulombic efficiency (CE) and safe hazards. Designing unique lithiophilic structure is an efficient strategy to control Li uniformly plating /stripping. Here, we report the silver (Ag) nanoparticles coated with nitrogen-doped onion-like carbon microspheres (Ag@NCS) as a host to reduce the nucleation overpotential of Li for dendrite-free LBMs. The Ag@NCS were prepared by a simple one-step injection pyrolysis. The lithiophilic Ag is demonstrated to be priority selective deposition of Li in the carbon cage. Meanwhile, the onion-like structure benefits to uniform lithium nucleation and dendrite-free lithium during cycling. Impressively, we successfully captured lithium metal on different hosts at atomic scale, further proving that Ag@NCS can effectively and uniformly deposit Li. Besides, Ag@NCS show a superiorly electrochemical performance with a low nucleation overpotential (∼1 mV), high CE and stable cycling performance (over 400 cycles at 0.5 mA cm^-2) compared to the Ag-free onion-like carbon in LMBs. Even under harsh conditions (1 mA cm^-2, 4 mA h cm^-2), Ag@NCS still present superior cycling stability for more than 150 cycles. Furthermore, a full cell composed of LiFePO₄ cathode exhibits significantly improved voltage hysteresis with low voltage polarization. This work provides a new choice and route for the design and preparation of lithiophilic host materials.