A binder-free nano sulfur-carbon nanotube composite material featured by clusters of sulfur nanocrystals anchored across the superaligned carbon nanotube (SACNT) matrix is fabricated via a facile solution-based method. The conductive SACNT matrix not only avoids self-aggregation and ensures dispersive distribution of the sulfur nanocrystals but also offers three-dimensional continuous electron pathway, provides sufficient porosity in the matrix to benefit electrolyte infiltration, confines the sulfur/polysulfides, and accommodates the volume variations of sulfur during cycling. The nanosized sulfur particles shorten lithium ion diffusion path, and the confinement of sulfur particles in the SACNT network guarantees the stability of structure and electrochemical performance of the composite. The nano S-SACNT composite cathode delivers an initial discharge capacity of 1071 mAh g(-1), a peak capacity of 1088 mAh g(-1), and capacity retention of 85% after 100 cycles with high Coulombic efficiency (∼100%) at 1 C. Moreover, at high current rates the nano S-SACNT composite displays impressive capacities of 1006 mAh g(-1) at 2 C, 960 mAh g(-1) at 5 C, and 879 mAh g(-1) at 10 C.

Ultrathin MnO 2 /graphene oxide/carbon nanotube (G/M@CNT) interlayers are developed as efficient polysulfide-trapping shields for high-performance Li-S batteries. A simple layer-by-layer procedure is used to construct a sandwiched vein-membrane interlayer of thickness 2 µm and areal density 0.104 mg cm −2 by loading MnO 2 nanoparticles and graphene oxide (GO) sheets on superaligned carbon nanotube films. The G/M@CNT interlayer provides a physical shield against both polysulfide shuttling and chemical adsorption of polysulfides by MnO 2 nanoparticles and GO sheets. The synergetic effect of the G/M@CNT interlayer enables the production of Li-S cells with high sulfur loadings (60-80 wt%), a low capacity decay rate (−0.029% per cycle over 2500 cycles at 1 C), high rate performance (747 mA h g −1 at a charge rate of 10 C), and a low self-discharge rate with high capacity retention (93.0% after 20 d rest). Electrochemical impedance spectroscopy, cyclic voltammetry, and scanning electron microscopy observations of the Li anodes after cycling confirm the polysulfide-trapping ability of the G/M@CNT interlayer and show its potential in developing high-performance Li-S batteries.

Sulfur-porous carbon nanotube (S-PCNT) composites are proposed as cathode materials for advanced lithium-sulfur (Li-S) batteries. Abundant mesopores are introduced to superaligned carbon nanotubes (SACNTs) through controlled oxidation in air to obtain porous carbon nanotubes (PCNTs). Compared to original SACNTs, improved dispersive behavior, enhanced conductivity, and higher mechanical strength are demonstrated in PCNTs. Meanwhile, high flexibility and sufficient intertube interaction are preserved in PCNTs to support binder-free and flexible electrodes. Additionally, several attractive features, including high surface area and abundant adsorption points on tubes, are introduced, which allow high sulfur loading, provide dual protection to sulfur cathode materials, and consequently alleviate the capacity fade especially during slow charge/discharge processes. When used as cathodes for Li-S batteries, a high sulfur loading of 60 wt % is achieved, with excellent reversible capacities of 866 and 526 mAh g(-1) based on the weights of sulfur and electrode, respectively, after 100 cycles at a slow charge/discharge rate of 0.1C, revealing efficient suppression of polysulfide dissolution. Even with a high sulfur loading of 70 wt %, the S-PCNT composite maintains capacities of 760 and 528 mAh g(-1) based on the weights of sulfur and electrode, respectively, after 100 cycles at 0.1C, outperforming the current state-of-the-art sulfur cathodes. Improved high-rate capability is also delivered by the S-PCNT composites, revealing their potentials as high-performance carbon-sulfur composite cathodes for Li-S batteries.

A multifunctional interlayer, composed of molybdenum diphosphide (MoP ) nanoparticles and a carbon nanotube (CNT) film, is introduced into a lithium-sulfur (Li-S) battery system to suppress polysulfide migration. Molybdenum diphosphide acts as the catalyst and can capture polysulfides and improve the polysulfide conversion activity during the discharge/charge processes. The CNT film acts as a conductive skeleton to support the MoP nanoparticles and to ensure their uniform distribution. The CNT film physically hinders polysulfide migration, acts as a current collector, and provides abundant electron pathways. The Li-S battery containing the multifunctional MoP /CNT interlayer exhibits excellent electrochemical performance. It delivers a reversible specific capacity of 905 mA h g over 100 cycles at 0.2 C, with a capacity decay of 0.152% per cycle. These results suggest the introduction of the multifunctional CNT/MoP interlayer as an effective and practical method for producing high-performance Li-S batteries.

A binder-free sulfur–carbon nanotube/graphene composite electrode is fabricated by a scalable ultrasonication-assisted method, demonstrating high capacity, reversibility, and rate capability.

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Mesoporous lithium titanate (LTO) nanoclusters are in situ synthesized in a network of super aligned carbon nanotubes (SACNTs) via a solution-based method followed by heat treatment in air. In the LTO-CNT composite, SACNTs not only serve as the skeleton to support a binder-free electrode, but also render the composite with high conductivity, flexibility, and mechanical strength. The homogeneously dispersed LTO nanoclusters among the SACNTs allow each LTO grain to effectively access the electrolyte and the conductive network, benefiting both ion and electron transport. By the incorporation of LTO into the CNT network, mechanical reinforcement is also achieved. When serving as a negative electrode for lithium ion batteries, such a robust composite-network architecture provides the electrodes with effective charge transport and structural integrity, leading to high-performance flexible electrodes with high capacity, high rate capability, and excellent cycling stability.