Lithium–sulfur batteries (Li–S) have become a viable alternative to future energy storage devices. The electrochemical reaction based on lithium and sulfur promises an extraordinary theoretical energy density, which is far higher than current commercialized Li-ion batteries. However, the principal disadvantage impeding the success of Li–S batteries lies in the severe leakage and migration of soluble lithium polysulfide intermediates out of cathodes upon cycling. The loss of active sulfur species incurs significant capacity decay and poor battery lifespans. Considerable efforts have been devoted to developing various sulfur host materials that can effectively anchor lithium polysulfides. Herein, a comprehensive review is presented of recent advances in sulfur host materials. On the basis of the electrochemistry of Li–S batteries, the strategies for anchoring polysulfides are systematically categorized into physical confinement and chemical bonding. The structural merits of various sulfur host materials are highlighted, and the interaction mechanisms with sulfur species are discussed in detail, which provides valuable insights into the rational design and engineering of advanced sulfur host materials facilitating the commercialization of Li–S batteries. Future challenges and promising research prospects for sulfur host materials are proposed at the end of the review.

Host Materials Anchoring Polysulfides in Li–S Batteries Reviewed

Introduction Lithium-sulfur batteries are considered as a promising candidate for next-generation secondary batteries because of their high theoretical capacit y, safe operating voltage (2.15 V vs. Li/Li ), and low cost. Nevertheless, lithium-sulfur batteries suffer from capacity fading, which limits their widespread application, due to the insulating nature of sulfur and its reduced pro ducts and the dissolution of intermediate lithium polysul fides. To address these problems, carbon-based materials have been integrated with sulfur to enhance the conductivity and inhibit the polysulfide dissolutio n. Recently, graphene, a single-atom-thick carbon mate rial with superior electrical conductivity and mechanica l flexibility, has been successfully applied in lithi um-sulfur batteries. While graphene-sulfur composite cathodes  demonstrate promising electrochemical performance, their synthesis is usually complicated and challeng ing for large-scale application. On the other hand, the sol utionbased synthesis without heat treatment produces lar ge crystalline sulfur particles, resulting in low util ization of active materials and poor rate performance. Herein, we report hydroxylated graphene nanosheets as a substr ate to produce graphene-amorphous sulfur nanocomposites, exhibiting superior cyclability at high rates, by a facile in situ deposition method at room temperature.

Hydroxylated Graphene-Sulfur Nanocomposites for High-Rate Lithium-Sulfur Batteries

A Review of Heteroatom Doped Materials for Advanced Lithium–Sulfur Batteries

The increasing demand for wearable electronic devices necessitates flexible batteries with high stability and desirable energy density. Flexible lithium-sulfur batteries (FLSBs) have been increasingly studied due to their high theoretical energy density through the multielectron chemistry of low-cost sulfur. However, the implementation of FLSBs is challenged by several obstacles, including their low practical energy density, short life, and poor flexibility. Various graphene-based materials have been applied to address these issues. Graphene, with good conductivity and flexibility, exhibits synergistic effects with other active/catalytic/flexible materials to form multifunctional graphene-based materials, which play a pivotal role in FLSBs. This review summarizes the recent progress of graphene-based materials that have been used as various FLSB components, including cathodes, interlayers, and anodes. Particular attention is focused on the precise nanostructures, graphene efficacy, interfacial effects, and battery layout for realizing FLSBs with good flexibility, energy density, and cycling stability.

Graphene-Based Materials for Flexible Lithium-Sulfur Batteries.

Aqueous zinc ion capacitors (ZICs) with hydrogel electrolytes (HEs), that afford the superiority of high sustainability, inherent safety, appealing energy/power densities, and extraordinary mechanics, have long been considered as an...

All-Around Supramolecular Zwitterionic Hydrogel Electrolytes Enabling Environmentally Adaptive Dendrite-Free Aqueous Zinc Ion Capacitors

Carbon materials have received considerable attention as host cathode materials for sulfur in lithium-sulfur batteries; N-doped carbon materials show particularly high electrocatalytic activity. Efforts are made to synthesize N-doped carbon materials by introducing nitrogen-rich sources followed by sintering or hydrothermal processes. In the present work, an in situ hollow cathode discharge plasma treatment method is used to prepare 3D porous frameworks based on N-doped graphene as a potential conductive matrix material. The resulting N-doped graphene is used to prepare a 3D porous framework with a S content of 90 wt% as a cathode in lithium-sulfur cells, which delivers a specific discharge capacity of 1186 mAh g-1 at 0.1 C, a coulombic efficiency of 96% after 200 cycles, and a capacity retention of 578 mAh g-1 at 1.0 C after 1000 cycles. The performance is attributed to the flexible 3D structure and clustering of pyridinic N-dopants in graphene. The N-doped graphene shows high electrochemical performance and the flexible 3D porous stable structure accommodates the considerable volume change of the active material during lithium insertion and extraction processes, improving the long-term electrochemical performance.

Plasma Treatment for Nitrogen-Doped 3D Graphene Framework by a Conductive Matrix with Sulfur for High-Performance Li-S Batteries.

Hydrogel electrolytes have attracted enormous attention in flexible and safe supercapacitors. However, the interfacial contact problem between hydrogel electrolyte and electrodes, and the environmental instability are the key factors restricting the development of hydrogel-based supercapacitors. Here, a nucleotide-tackified adhesive organohydrogel electrolyte is successfully constructed and exhibits freezing resistance and water-holding ability based on the water/glycerol binary solvent system. Adenosine monophosphate enables the organohydrogels to possess outstanding adhesion and mechanical robustness. The robust adhesion can ensure close contact between the organohydrogel electrolyte and electrodes for constructing an all-in-one supercapacitor with low interfacial contact resistance. Impressively, the integrated organohydrogel-based supercapacitors display an areal specific capacitance of 163.6 mF cm-2 . Besides, the supercapacitors feature prominent environmental stability with capacitance retention of 90.6% after 5000 charging/discharging cycles at -20 °C. Furthermore, based on the strong interfacial adhesion, the supercapacitors present excellent electrochemical stability without delamination/displacement between electrolyte and electrodes even under severe deformations such as bending and twisting. It is anticipated that this work will provide an encouraging way for developing flexible energy storage devices with electrochemical stability and environmental adaptability.

Nucleotide-Tackified Organohydrogel Electrolyte for Environmentally Self-Adaptive Flexible Supercapacitor with Robust Electrolyte/Electrode Interface.

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Plasma Treatment for Nitrogen-Doped 3D Graphene Framework by a Conductive Matrix with Sulfur for High-Performance Li-S Batteries.

Nucleotide-Tackified Organohydrogel Electrolyte for Environmentally Self-Adaptive Flexible Supercapacitor with Robust Electrolyte/Electrode Interface.