Coupling a Sponge Metal Fibers Skeleton with In Situ Surface Engineering to Achieve Advanced Electrodes for Flexible Lithium-Sulfur Batteries

Lithium-sulfur batteries (LSBs) are regarded as promising next-generation energy storage systems, however, the uncontrollable dendrite formation and serious polysulfide shuttling severely hinder their commercial success. Herein, a powerful 3D sponge nickel (SN) skeleton plus in situ surface engineering strategy, to address these issues synergistically, is reported, and a high-performance flexible LSB device is constructed. Specifically, the rationally designed spray-quenched lithium metal on the SN matrix (solid electrolyte interface (SEI)@Li/SN), as dendrite inhibitor, combines the merits of the 3D lithiophilic SN skeleton and the in situ formed SEI layer derived from the spray-quenching process, and thereby exhibits a steady overpotential within 75 mV for 1500 h at 5 mA cm^-2 /10 mA h cm^-2 . Meanwhile, in situ surface sulfurization of the SN skeleton hybridizing with the carbon/sulfur composite (SC@Ni₃ S₂ /SN) serves as efficient lithium polysulfide adsorbent to catalyze the overall reaction kinetics. COMSOL Multiphysics simulations and density functional theory calculations are further conducted to explore the underlying mechanisms. As a proof of concept, the well-designed SEI@Li/SN||SC@Ni₃ S₂ /SN full cell shows excellent electrochemical performance with a negative/positive ratio in capacity of ≈2 and capacity retention of 99.82% at 1 C under mechanical deformation. The novel design principles of these materials and electrodes successfully shed new light on the development of flexible LSBs.