The notorious dendrite and infinite volume change seriously restrict the advancement of lithium metal anodes (LMAs), during the long-term process of stripping/plating. Herein, the nanosheets of metal fluoride (CoF₂) and metal nitride (CoN) with magnificent lithiophilicity on the nickel (Ni) foam are designed as the “regulator” to uniform the Li plating and build stronger solid electrolyte interface (SEI) layer for dendrite free LMAs. The Ni foam offers abundant space to receive deposited Li metal. The CoN nanosheets can guarantee the fast transfer of electrons, which provides a stable interface of Li⁺ reduction. Moreover, the nanosheet structure with lithiophilicity would accelerate the move of Li⁺ and decrease the nucleation barrier, due to the high lattice-matching of Li and CoN. Meanwhile, the CoF₂ could increase the content of F (LiF) in the SEI layer, which enhances the strength and avoids the destruction of SEI layer. With the cooperation of CoN and CoF₂, the composited anode (Li/NF@CNCF) exhibits ultra-long cycle performance (more than 1200 h) and fantastic structure stability at 1 mA·cm⁻² with 1 mAh·cm⁻². Based on the LiFePO₄ and Li/NF@CNCF, the full cells deliver excellent specifical capacity and steady coulombic efficiency. The strategy contributes an effective approach to alleviate the issues of lithium metal anodes in the field of LMAs.

Oxygen vacancy (Vö) is important in the modification of electrode for rechargeable batteries. However, due to the scarcity of suitable preparation strategy with controllable Vö incorporation, the impact of Vö concentration on the electrochemical performances remains unclear. Thus, in this work, Vö-V₂O₅-PEDOT (VöVP) with tunable Vö concentration is achieved via a spontaneous polymerization strategy, with the capability of mass-production. The introduction of poly(2,3-dihydrothieno-1,4-dioxin) (PEDOT) not only leads to the formation of Vö in V₂O₅, but it also results in a larger interlayer spacing. The as-prepared Vö-V₂O₅-PEDOT-20.3% with Vö concentration of 20.3% (denoted as VöVP-20) is able to exhibit high capacity of 449 mAh·g⁻¹ at current density of 0.2 A·g⁻¹, with excellent cyclic performance of 94.3% after 6,000 cycles. It is shown in the theoretical calculations that excessive Vö in V₂O₅ will lead to an increase in the band gap, which inhibits the electrochemical kinetics and charge conductivity. This is further demonstrated in the experimental results as the electrochemical performance starts to decline when Vö concentration increases beyond 20.3%. Thus, based on this work, scalable fabrication of high-performance electrode with tunable Vö concentration can be achieved with the proposed strategy.