Monolayer Amorphous Carbon: Unlocking Disorder‐Induced Lithiophilicity

Atomic‐scale disorder in monolayer amorphous carbon generates abundant Li binding sites. Combined contact angle, electrochemical, and Density Functional Theory analyses show how this broad distribution of binding energies lowers the contact angle to around 30°, reduces the nucleation overpotential, and yields uniform lithium deposition. The study establishes disorder‐tuned two‐dimensional amorphous carbon as a route to controlled metal nucleation. Abstract Dendritic lithium growth on the current collector remains a major obstacle to developing anode‐less batteries, arising from inhomogeneous lithium nucleation and uneven surface lithiophilicity. Existing approaches, such as metallic or carbonaceous interlayers, often fail to stabilize lithium deposition due to mechanical degradation or spatial variations in lithium affinity. Here, we demonstrate that a monolayer amorphous carbon (MAC) film—a single‐atom‐thick disordered sp2 network grown directly on copper—can fundamentally alter lithium nucleation behavior. The topological disorder of MAC produces a dense distribution of electron‐rich sites that uniformly strengthen lithium binding. As a result, the MAC surface exhibits a lithium contact angle of 31 ± 5°, four times lower than that of graphene and nearly three times lower than that of bare copper, leading to homogeneous wetting and deposition. Electrochemical tests reveal a reduced nucleation overpotential of 28.9 mV at 0.5 mA cm−2. Density functional theory and scanning tunneling microscopy confirm that disorder‐induced localization of states near the Fermi level enhances electronegativity and forms continuous lithium‐binding sites. These findings establish intrinsic structural disorder, rather than chemical doping, as an effective route to designing uniformly lithiophilic current collectors for next‐generation anode‐less batteries. Atomic-scale disorder in monolayer amorphous carbon generates abundant Li binding sites. Combined contact angle, electrochemical, and Density Functional Theory analyses show how this broad distribution of binding energies lowers the contact angle to around 30°, reduces the nucleation overpotential, and yields uniform lithium deposition. The study establishes disorder-tuned two-dimensional amorphous carbon as a route to controlled metal nucleation. Abstract Dendritic lithium growth on the current collector remains a major obstacle to developing anode-less batteries, arising from inhomogeneous lithium nucleation and uneven surface lithiophilicity. Existing approaches, such as metallic or carbonaceous interlayers, often fail to stabilize lithium deposition due to mechanical degradation or spatial variations in lithium affinity. Here, we demonstrate that a monolayer amorphous carbon (MAC) film—a single-atom-thick disordered sp 2 network grown directly on copper—can fundamentally alter lithium nucleation behavior. The topological disorder of MAC produces a dense distribution of electron-rich sites that uniformly strengthen lithium binding. As a result, the MAC surface exhibits a lithium contact angle of 31 ± 5°, four times lower than that of graphene and nearly three times lower than that of bare copper, leading to homogeneous wetting and deposition. Electrochemical tests reveal a reduced nucleation overpotential of 28.9 mV at 0.5 mA cm −2. Density functional theory and scanning tunneling microscopy confirm that disorder-induced localization of states near the Fermi level enhances electronegativity and forms continuous lithium-binding sites. These findings establish intrinsic structural disorder, rather than chemical doping, as an effective route to designing uniformly lithiophilic current collectors for next-generation anode-less batteries. Advanced Science, EarlyView.