Polydopamine architectured stable layered MnO2 for dendrite free lithium metal batteries

Lithium metal, a widely recognized anode material for next generation high energy density batteries, is hindered by challenges such as dendrite growth and interfacial instability. Lithiophilic MnO 2 based current collectors have demonstrated potential in regulating lithium deposition. However, the critical relationship between MnO 2 phase selection, structural stability, and electrochemical performance remains poorly understood. In this study, we employ density functional theory (DFT) calculations to guide the fabrication of MnO 2 based current collectors, followed by a dual functional modification strategy through reductive and conductive polydopamine (PDA) integration. This approach synergistically enhances both the electronic conductivity and structural stability of δ-MnO 2 . The reductive nature of PDA induces partial conversion of Mn 4+ to Mn 2+ , generating oxygen vacancies (Ovs) that facilitate Li + diffusion, while its conjugated polymer framework significantly improves electrical conductivity. The optimized electrode achieves uniform lithium deposition with an average coulombic efficiency (CE) of 98.5% over 300 cycles at 1 mA cm −2 . This work presents a novel theoretical and experimental approach to designing durable, dendrite suppressing current collectors, representing a significant step toward practical lithium metal batteries.