Porous transition metal oxide scaffold implanted with interpenetrated catalytic network enabling polysulfides restricted and dendrite free Lithium–Sulfur batteries

“Rigid” 3D porous Co-TiO 2 framework in-situ implanted with Co nanoparticles encapsulated N-doped CNTs are designed as efficient dual-functional hosts for both sulfur-cathode and lithium-anode in lithium-sulfur batteries. The polysulfides “shuttle effect” and lithium dendrite growth are simultaneously alleviated thanks to the unique structure and adsorption/catalytic/lithophilic characteristics of the desired material. Excellent cycling stability along with electrochemical properties are achieved by the full lithium-sulfur batteries. • Co-TiO 2 with a 3DOM structure is used as stable skeleton for both S and Li hosts. • Co@NCNTs are grown in-situ on 3DOM Co-TiO 2 to boost conductivity/catalytic ability. • Interpenetrated NCNTs network boosts the holistic conductivity. • Co NPs improve LiPS/Li + conversion due to integrated catalytic/lithophilic nature. • Li–S full cell shows super capacity/rate property and stability at lean electrolyte. The exploration of porous polar hosts with good structural stability, high catalytic activity, lithophilic nature, and high-conductivity is desirable to solve the dilatory polysulfide redox kinetics and the uncontrolled lithium dendrite growth for efficient and stable lithium–sulfur (Li–S) batteries. Herein, a novel hierarchical metal oxide-based scaffold is developed, in which N-doped carbon nanotubes encapsulated with Co nanoparticles are in-situ implanted within three-dimensional ordered macroporous Co-doped TiO 2 (Co@NCNTs/Co-TiO 2 ) as efficient hosts for both sulfur and Li electrodes. Benefiting from the excellent stability of polar Co-TiO 2 skeleton, high catalytic activity and lithophilic properties of Co nanoparticles, and high-conductivity of the inter-penetrated NCNTs, the polysulfide conversion kinetics are dramatically boosted, and the dendrite-free lithium electrochemistry is simultaneously accomplished. Cooperatively, the Co@NCNTs/Co-TiO 2 /Li ‖ Co@NCNTs/Co-TiO 2 /S full cell expresses high rate capability of 879.66 mAh g −1 at 5C, as well as super cycling stability with a low capacity decay rate of about 0.033% after 1000 cycles at 3C. Additionally, Li–S pouch cell assembled by Co@NCNTs/Co-TiO 2 /Li anode and Co@NCNTs/Co-TiO 2 /S cathode also exhibits a remarkable discharge capacity of 1020.4 mAh g −1 with sulfur loading even reaching 4.5 mg cm −2 after 200 cycles. The present work reveals an effective strategy for developing advanced Li–S batteries dual-functional electrodes.