Lithium-ion batteries, which have revolutionized portable electronics over the past three decades, were eventually recognized with the 2019 Nobel Prize in chemistry. As the energy density of current lithium-ion batteries is approaching its limit, developing new battery technologies beyond lithium-ion chemistry is significant for next-generation high energy storage. Lithium-sulfur (Li-S) batteries, which rely on the reversible redox reactions between lithium and sulfur, appears to be a promising energy storage system to take over from the conventional lithium-ion batteries for next-generation energy storage owing to their overwhelming energy density compared to the existing lithium-ion batteries today. Over the past 60 years, especially the past decade, significant academic and commercial progress has been made on Li-S batteries. From the concept of the sulfur cathode first proposed in the 1960s to the current commercial Li-S batteries used in unmanned aircraft, the story of Li-S batteries is full of breakthroughs and back tracing steps. Herein, the development and advancement of Li-S batteries in terms of sulfur-based composite cathode design, separator modification, binder improvement, electrolyte optimization, and lithium metal protection is summarized. An outlook on the future directions and prospects for Li-S batteries is also offered.

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

Lithium-sulfur (Li-S) batteries have a high specific energy capacity and density of 1675 mAh g-1 and 2670 Wh kg-1 , respectively, rendering them among the most promising successors for lithium-ion batteries. However, there are myriads of obstacles in the practical application and commercialization of Li-S batteries, including the low conductivity of sulfur and its discharge products (Li2 S/Li2 S2 ), volume expansion of sulfur electrode, and the polysulfide shuttle effect. Hence, immense attention has been devoted to rectifying these issues, of which the application of metal-based compounds (i.e., transition metal, metal phosphides, sulfides, oxides, carbides, nitrides, phosphosulfides, MXenes, hydroxides, and metal-organic frameworks) as sulfur hosts is profiled as a fascinating strategy to hinder the polysulfide shuttle effect stemming from the polar-polar interactions between the metal compounds and polysulfides. This review encompasses the fundamental electrochemical principles of Li-S batteries and insights into the interactions between the metal-based compounds and the polysulfides, with emphasis on the intimate structure-activity relationship corroborated with theoretical calculations. Additionally, the integration of conductive carbon-based materials to ameliorate the existing adsorptive abilities of the metal-based compound is systematically discussed. Lastly, the challenges and prospects toward the smart design of catalysts for the future development of practical Li-S batteries are presented.

Lithium–Sulfur Battery Cathode Design: Tailoring Metal-Based Nanostructures for Robust Polysulfide Adsorption and Catalytic Conversion

Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives

Covalent organic frameworks (COF) possess a robust and porous crystalline structure, making them an appealing candidate for energy storage. Herein, we report an exfoliated polyimide COF composite (P-COF@SWCNT) prepared by an in situ condensation of anhydride and amine on the single-walled carbon nanotubes as advanced anode for potassium-ion batteries (PIBs). Numerous active sites exposed on the exfoliated frameworks and the various open pathways promote the highly efficient ion diffusion in the P-COF@SWCNT while preventing irreversible dissolution in the electrolyte. During the charging/discharging process, K+ is engaged in the carbonyls of imide group and naphthalene rings through the enolization and π-K+ effect, which is demonstrated by the DFT calculation and XPS, ex-situ FTIR, Raman. As a result, the prepared P-COF@SWCNT anode enables an incredibly high reversible specific capacity of 438 mA h g-1 at 0.05 A g-1 and extended stability. The structural advantage of P-COF@SWCNT enables more insights into the design and versatility of COF as an electrode. 

Covalent Organic Framework with Highly Accessible Carbonyls and π‐Cation Effect for Advanced Potassium‐Ion Batteries

Lithium-sulfur (Li-S) batteries are promising candidates for next-generation energy storage, yet they are plagued by the notorious polysulfide shuttle effect and sluggish redox kinetics. While rationally designed redox mediators can facilitate polysulfide conversion, favorable bidirectional sulfur electrocatalysis remains a formidable challenge. Herein, selective dual-defect engineering (i.e., introducing both N-doping and Se-vacancies) of a common MoSe2 electrocatalyst is used to manipulate the bidirectional Li2 S redox. Systematic theoretical prediction and detailed electrokinetic analysis reveal the selective electrocatalytic effect of the two types of defects, thereby achieving a deeper mechanistic understanding of the bidirectional sulfur electrochemistry. The Li-S battery using this electrocatalyst exhibits excellent cyclability, with a low capacity decay rate of 0.04% per cycle over 1000 cycles at 2.0 C. More impressively, the potential for practical applications is highlighted by a high areal capacity (7.3 mAh cm-2 ) and the construction of a flexible pouch cell. Such selective electrocatalysis created by dual-defect engineering is an appealing approach toward working Li-S systems.

Manipulating Electrocatalytic Li2S Redox via Selective Dual-Defect Engineering for Li–S Batteries

Electrocatalysts remain vitally important for the rational management of intermediate polysulfides (LiPSs) in the realm of Li-S batteries. In terms of transition-metal-based candidates, in situ evolution of electrocatalysts in the course of an electrochemical process has been acknowledged; nevertheless, consensus has not yet been reached on their real functional states as well as catalytic mechanisms. Herein, we report an all-chemical vapor deposition design of the defective vanadium diselenide (VSe2)-vertical graphene (VG) heterostructure on carbon cloth (CC) targeting a high-performance sulfur host. The electrochemistry induces the sulfurization of VSe2 to VS2 at Se vacancy sites, which propels the adsorption and conversion of LiPSs. Accordingly, the VSe2-VG@CC/S electrode harvests an excellent cycling stability at 5.0 C with a capacity decay of only 0.039% per cycle over 800 cycles, accompanied by a high areal capacity of 4.9 mAh cm-2 under an elevated sulfur loading of 9.6 mg cm-2. Theoretical simulation combined with operando characterizations reveals the key role played by the Se vacancy with respect to the electrocatalyst evolution and LiPS regulation. This work offers insight into the rational design of heterostructure sulfur hosts throughout defect engineering.

Defective VSe2-Graphene Heterostructures Enabling In Situ Electrocatalyst Evolution for Lithium-Sulfur Batteries.

Harmonized edge/graphitic-nitrogen doped carbon nanopolyhedron@nanosheet composite via salt-confined strategy for advanced K-ion hybrid capacitors

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Defective VSe2-Graphene Heterostructures Enabling In Situ Electrocatalyst Evolution for Lithium-Sulfur Batteries.

Harmonized edge/graphitic-nitrogen doped carbon nanopolyhedron@nanosheet composite via salt-confined strategy for advanced K-ion hybrid capacitors