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Highlights: The robust organic/inorganic hybrid interlayer derived from in situ formed tribofilms were fabricated by using a scalable rolling method. The interlayer facilitates dendrite-free lithium metal anodes by building local de-solvation environments near the interface and inhibiting both dendrite growth and electrolytes corrosion. The symmetrical cell exhibits a remarkable lifespan of 5,600 h (1.0 mA cm-2 and 1.0 mAh cm-2) and 1,350 cycles even at a harsh condition (18.0 mA cm-2 and 3.0 mAh cm-2). The practical application of Li metal anodes (LMAs) is limited by uncontrolled dendrite growth and side reactions. Herein, we propose a new friction-induced strategy to produce high-performance thin Li anode (Li@CFO). By virtue of the in situ friction reaction between fluoropolymer grease and Li strips during rolling, a robust organic/inorganic hybrid interlayer (lithiophilic LiF/LiC6 framework hybridized -CF2-O-CF2- chains) was formed atop Li metal. The derived interface contributes to reversible Li plating/stripping behaviors by mitigating side reactions and decreasing the solvation degree at the interface. The Li@CFO||Li@CFO symmetrical cell exhibits a remarkable lifespan for 5,600 h (1.0 mA cm−2 and 1.0 mAh cm−2) and 1,350 cycles even at a harsh condition (18.0 mA cm−2 and 3.0 mAh cm−2). When paired with high-loading LiFePO4 cathodes, the full cell lasts over 450 cycles at 1C with a high-capacity retention of 99.9%. This work provides a new friction-induced strategy for producing high-performance thin LMAs. [ABSTRACT FROM AUTHOR]

The Zn metal anode is subject to uncontrolled dendrites and parasitic reactions, which often require a big thickness of Zn foil, resulting in excess capacity and extremely low utilization. Here, an ultrathin Zn composite anode (24 µm) is developed with a protective hydrophobic layer (covalent (C2F4)n chains and F‐doped carbonized ingredient) constructed on Cu foil (denoted as (C2F4)n‐C@Cu) as a host by one‐step pyrolytic evaporation deposition. The repulsion of (C2F4)n to Zn2+ makes the (C2F4)n‐C@Cu interface possess enhanced adsorption ability, driving more charge transfer under the layer. With its good hydrophobicity, this layer prevents H2O from damaging the plated Zn. Combined with the semi‐ionic‐state fluorine as zincophilic site, the host guides uniform and dense Zn deposition for making ultrathin Zn anode. As a result, the (C2F4)n‐C@Cu electrode exhibits high average CE of 99.6% over 3000 cycles at 2 mA cm−2. Benchmarked against the commercial 20µm‐Zn foil, the (C2F4)n‐C@Cu@Zn anode achieves enhanced stability (1200 h at 1 mA cm−2), only 100 h for the 20µm‐Zn foil. When paired with V2O5 cathode, the Zn composite anode makes the full cell deliver 88% retention for 2500 cycles. [ABSTRACT FROM AUTHOR]

Lithium metal anode generally shows poor humid air stability and unsatisfied cycling lifespan, which poses significant challenges for practical productions and applications. Herein, a highly hydrophobic and dendrite-free lithium anode (Li@FC) was fabricated by coating fluorinated carbon (FC) layers on the surface. The Li@FC anode shows improved stability against humid environments with a large contact angle of 139° due to the formation of hydrophobic interfacial layers consisting of fluorinated carbon, and FC derived carbon matrix and LiF nanocrystals. More importantly, LiF possesses high Li+ conductive ability while conductive carbon matrix can provide lithiophilic host for lithium deposition. The Li@FC anode suppresses the formation of lithium dendrites by orienting lithium deposition. As a result, Li@FC anode exhibits excellent electrochemical performances in both symmetric cells and LiFePO 4 full cells. This design offers a potential approach for developing lithium metal anodes that are both air-stable and dendrite-free, thereby enhancing the reliability of lithium metal batteries. [Display omitted] • Fluorinated carbon derived coatings enable hydrophobic/dendrite-free lithium anodes. • Interfacial layers consist of fluorinated carbon, carbon matrix and LiF nanocrystals. • Highly conductive LiF and lithiophilic carbon matrix facilitate reversible plating. • The Li@FC anode exhibits excellent performances by inhibiting Li dendrite growth. [ABSTRACT FROM AUTHOR]