Free-Standing Binder-Free Cellulose-Based MoS₂@C@CNFs Electrodes for Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries are promising high-energy systems but suffer from the polysulfide shuttle effect, low sulfur conductivity, and large volume expansions. Herein, we report a novel, free-standing, binder-free sulfur host composed of hierarchical MoS₂ and carbon nanoparticle decorated cellulose-based CNFs (MoS₂@C@CNFs) for Li–S batteries for the first time. It is fabricated via electrospinning, carbon coating, carbonization, and hydrothermal methods. Carbon-coated CNFs promote high active material loading and Li-ion transport, while MoS₂ nanosheets anchored on C@CNFs further increase the surface area and provide abundant active sites. The hierarchical structure, consisting of 2D layered MoS₂ nanosheets and 0D carbon nanoparticles integrated onto the surface of 1D porous CNFs, creates a multiscale network that enhances reaction kinetics and electrical conductivity, mitigates the shuttle effect, and accommodates sulfur volume expansion. MoS₂@C@CNFs cathode shows excellent electrochemical performance, delivering an initial capacity of 1320 mA h g⁻¹ at 0.2C, and a reversible capacity of 1050 mA h g⁻¹ after 250 cycles, with a capacity retention of 79.55%. After 450 cycles at 2C, it exhibits a low average capacity fading rate of 0.0885% per cycle. This study offers a novel strategy to produce free-standing binder-free cellulose-based CNF electrodes for high-performance Li–S batteries.