Lithium–sulfur (Li–S) batteries are regarded as the most promising next‐generation energy storage systems due to their high energy density and cost‐effectiveness. However, their practical applications are seriously hindered by several inevitable drawbacks, especially the shuttle effects of soluble lithium polysulfides (LiPSs) which lead to rapid capacity decay and short cycling lifespan. This review specifically concentrates on the shuttle path of LiPSs and their interaction with the corresponding cell components along the moving way, systematically retrospect the recent advances and strategies toward polysulfides diffusion suppression. Overall, the strategies for the shuttle effect inhibition can be classified into four parts, including capturing the LiPSs in the sulfur cathode, reducing the dissolution in electrolytes, blocking the shuttle channels by functional separators, and preventing the chemical reaction between LiPSs and Li metal anode. Herein, the fundamental aspect of Li–S batteries is introduced first to give an in‐deep understanding of the generation and shuttle effect of LiPSs. Then, the corresponding strategies toward LiPSs shuttle inhibition along the diffusion path are discussed step by step. Finally, general conclusions and perspectives for future research on shuttle issues and practical application of Li–S batteries are proposed.

Mixed transition metal sulfides with hollow structures hold great promise for energy-related applications. However, most of them are in the powder form, which should be mixed with unwanted polymer binders and conductive agents. In this study, a facile two-step strategy has been developed to grow mesoporous and hollow Ni-Zn-Co-S nanosword arrays (NSAs) on a nickel foam (NF) substrate with robust adhesion, which involves the hydrothermal growth of bimetallic Zn-Co-ZIF NSAs on NF and subsequent transformation into hollow Ni-Zn-Co-S NSAs through the sulfurization process. Benefiting from the unique structural and compositional advantages as well as directly grown conductive substrate, the Ni-Zn-Co-S-0.33 NSAs/NF electrode exhibits the best electrochemical performance when investigated as a binder-free electrode for supercapacitors. Impressively, the Ni-Zn-Co-S-0.33 NSAs/NF electrode delivers a high areal capacity of 1.11 mA h cm at the current density of 10 mA cm, and the corresponding specific capacity is as high as 358.1 mA h g. Moreover, an asymmetric supercapacitor (ASC) device based on the Ni-Zn-Co-S-0.33 NSAs/NF as the positive electrode and BiO/NF as the negative electrode has been successfully fabricated, and can deliver a high energy density of 91.7 W h kg at a power density of 458 W kg and maintain the energy density of 66.9 W h kg at a high power density of 6696 W kg. The electrochemical results suggest that the hollow Ni-Zn-Co-S NSAs would possess great potential for applications in high-performance supercapacitors.

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most widely and regarded as potential candidates, considering their higher theoretical gravimetric energy density (Li-S: 2615 Wh kg −1 , Na-S: 1673 Wh kg −1 ) than that of Li-ion (Lithium ion) batteries. [2] Despite possessing about twice the theoretical gravimetric and volumetric energy densities of Na-S batteries (Figure 1b), the sustainable development of Li-S batteries is still constrained by the low earth abundance (0.0017 wt%) and the resultant fastly rising price of lithium (Li) source. [3] Not only that, the main Li source, lithium carbonate, is usually prepared by the single production method, which is highly dependent on salt lake brines concentrated in South America geographically. [4] In sharp contrast, sodium (Na) sources are abundant (2.3 wt%) and scattered all over the world, as well as they can be prepared industrially in various ways, which will bring economic benefits. Therefore, although no substantial improvements in energy density and long-term durability are realized via switching to Na as the Li alternative in metal-sulfur batteries, developing Na-S batteries is more available for mitigating geostrategic and geo-economic competition and solving long-term energy bottlenecks in terms of technoeconomics. [3,5] Moreover, different from Li metal possessing high reaction activity to aluminum (Al), Na metal anode does not react with Al so that light and cheap Al foil can be used as the alternative anode current collector to Cu counterpart in the Na-S system, which could heighten gravimetric energy density and reduce cost, especially in pouch cells.Both Li and Na are alkali metals and have body-centered cubic crystal structures. These similarities in fundamental characteristics make Na metal possess similar physical and chemical properties to Li metal, such as high reaction activity, low melt temperature, vulnerability to the plastic deformation below the low yield strength, on the other hand, cause similar issues when Na or Li metal anodes are coupled with S cathode to assemble metal-sulfur batteries. [5] Subjected to the imperfection of alkali anode and S cathode, several similar challenges must be overcome for the practical application of Li-S and Na-S batteries, including uncontrollable growth of Li or Na dendrites, unstable solid electrolyte interface (SEI) layer on the surface of the anode, sluggish conversion kinetics between S active material and polysulfide intermediates, the dissolution and shuttle Metal-sulfur batteries exhibit great potential as next-generation rechargeable batteries due to the low sulfur cost and high theoretical energy density. Sodium-sulfur (Na-S) batteries present higher feasibility of long-term development than lithium-sulfur (Li-S) batteries in technoeconomic and geopolitical terms. Both lithium and sodium are alkali metal elements with body-centered cubic structures, leading to similar physical and chemical properties and exposing similar issues when employed as the anode in metal-sulfur batteries. Indeed, some inspiration for mechanism researches and strategies ...

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The commercial viability of lithium–sulfur batteries is still challenged by the notorious lithium polysulfides (LiPSs) shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode. Herein, a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton (3DIO FCSe-QDs@NC) is elaborately designed for both sulfur cathode and Li metal anode. The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble LiPSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors. Simultaneously, the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites. Taking advantage of these merits, the assembled Li–S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability (a low decay rate of 0.014% over 2,000 cycles at 2C). Remarkably, a promising areal capacity of 8.41 mAh cm−2 can be achieved at the sulfur loading up to 8.50 mg cm−2 with an ultra-low electrolyte/sulfur ratio of 4.1 μL mg−1. This work paves the bi-serve host design from systematic experimental and theoretical analysis, which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li–S full batteries.

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