Oxygenated lithiophilic interfaces in scalable nickel scaffolds toward stable and dendrite-free lithium metal batteries

Abstract

Lithium metal is a highly promising anode for next-generation rechargeable batteries due to its ultrahigh theoretical capacity (3860 mAh g−1) and the lowest electrochemical potential (−3.04 V vs. SHE). However, its practical application is hindered by dendritic growth, unstable solid electrolyte interphase (SEI), and electrically isolated “dead” lithium, which degrade cycling performance and safety. To mitigate these issues by lowering the local current density, three-dimensional (3D) porous scaffolds have been explored, yet their effectiveness remains limited due to the intrinsically lithiophobic nature of scaffold surfaces. Here, we present a facile and scalable strategy to construct 3D nickel scaffolds (NiOSc-400) with an oxygen-rich, lithiophilic NiO interface, using a two-step tunable surface modification route. NiOSc-400 promotes uniform Li+ adsorption and nucleation, while facilitating the in-situ formation of a Li2O-based quasi-SEI via a conversion reaction. NiOSc-400 exhibits excellent cycling stability with a Coulombic efficiency of 99.9% over 800 cycles at 0.5 mA cm−2 and maintains a low overpotential of 28.9 mV at 15 mA cm−2. This work provides a practically viable platform for dendrite-free, high-performance lithium metal anodes by rationally engineering interfacial chemistry and scaffold architecture.