Lithium–sulfur (Li–S) batteries have been considered as promising battery systems due to their huge advantages on theoretical energy density and rich resources. However, the shuttle effect and sluggish transformation of soluble lithium polysulfides (LiPSs) hinder the practical application of Li–S batteries. Tremendous sulfur host materials with unique catalytic activity have been exploited to inhibit the shuttle effect and accelerate LiPSs redox reactions, in which theoretical simulations have been widely adopted. This review aims to summarize the fundamentals and applications of theoretical models in sulfur cathodes. Concretely, the integration of theoretical models provides insights into the adsorption and conversion mechanisms of LiPSs and is further utilized in the smart design of catalysts for the exploitation of practical Li–S batteries. Finally, a perspective on the future combination of calculation technology and theoretical models is provided. 

A review on theoretical models for lithium–sulfur battery cathodes

The severe shuttle effect of polysulfides and sluggish redox kinetics are the main problems that hinder the practical applications of lithium–sulfur (Li–S) batteries. In this study, dual metallic single atom pairs are implanted into carbon nanospheres to address the shuttle effect and facilitate the bi-directional redox kinetics of sulfur. Fe sites are found to be favorable for the reduction reaction of polysulfides, while Co sites facilitate the dissolution of Li2S experimentally and theoretically, promoting the overall electrochemical performance of Li−S batteries due to the synergetic effect. The sulfur cathode with the dual metallic single atom pairs exhibits an ultrahigh capacity retention of 96.4% after 100 cycles at 0.5 C. More importantly, it demonstrates excellent rate performance (618 mAh g−1 at current density of 10 C) and outstanding cycle performance at 2 C after 2800 cycles with only 0.01% decay per cycle. Impressively, the assembled pouch cell delivers a high discharge capacity of 1385 mAh g−1 and retains 869 mAh g−1 after 100 cycles at 0.2 C. These results demonstrate the potential of dual single atom catalysts for the favorable bi-directional redox kinetics in Li−S batteries. 

Boosting Bi‐Directional Redox of Sulfur with Dual Metal Single Atom Pairs in Carbon Spheres Toward High‐Rate and Long‐Cycling Lithium–Sulfur Battery

Lithium–sulfur (Li–S) batteries are regarded as promising candidates for next‐generation energy storage systems. However, the slow kinetics and shuttle effects of polysulfides hinder their practical applications. Designing high‐efficiency catalysts to enhance the kinetics and suppress shuttling is one major task for the building of durable Li–S batteries. Here, a Co/CoSe junction is reported to catalyzepolysulfide conversion efficiently because the junction has metallic electron mobility and field‐enhanced catalytic activity. The mechanistic investigation reveals that the difference in the work functions of Co and CoSe rearranges the charge distribution in the junction and strengthens the interaction between polysulfides and CoSe, thereby yielding high catalytic activity. In addition, the relative stability of CoSe, as compared to Co, renders the junction durable upon cycling; therefore, demonstrating long‐term catalytic activity. Such a junction makes full use of metal‐like conductivity and field‐enhanced catalysis and provides an alternative approach to enhancing the catalytic conversion of polysulfides.

Co/CoSe Junctions Enable Efficient and Durable Electrocatalytic Conversion of Polysulfides for High‐Performance Li–S Batteries

Lithium–sulfur batteries (Li–S) are recognized as the next generation of secondary batteries due to their satisfactory theoretical specific capacity and energy density. However, a series of problems such as disordered migration behavior, sluggish redox kinetics, and serious shuttle effect of lithium polysulfides (LiPSs) greatly limit the commercial application. Herein, nanoreactors encapsulate heterostructure to guarantee sulfur conversion in the hosts where the heterostructure consists of FeP with moderate adsorption ability, excellent catalytic active and low work function, and Fe3O4 with strong adsorption ability and high work function. This rational configuration of heterostructure controls the direction of the interface built‐in electric field (BIEF) between catalyst and adsorbent, realizing the successive “trapping‐directional migration‐conversion” reaction mechanism to sulfur species. Thanks to BIEF as a bridge to connect the trapping site and catalytic site, Fe3O4/FeP@C─S cathode delivers an ultrahigh initial specific capacity of 1402 mAh g−1 at 0.1 C and remains more than 450 mAh g−1 at 5 C after 350 cycles. Even with a sulfur loading of 5.20 mg cm−2, it displayed the initial specific capacity of 970 mAh g−1. This work provided an effective strategy to design high‐performance electrocatalysts for commercial Li–S batteries.

Nanoreactors Encapsulating Built‐in Electric Field as a “Bridge” for Li–S Batteries: Directional Migration and Rapid Conversion of Polysulfides

Lithium−sulfur (Li−S) batteries with ultrahigh theoretical energy densities have thus far attracted significant attention as the next‐generation energy storage systems. However, the presence of the polysulfide shuttle effect and sluggish reaction kinetics have critically hindered their research progress. Herein, the fabrication of novel VC‐VO heterogeneous particles supported on a hierarchical porous carbon matrix (VC‐VO/HPC) is reported that regulate the disordered motion of lithium polysulfides (LiPSs); these particles can simultaneously achieve powerful anchoring, fast diffusion, and high‐efficiency conversion of LiPSs. Moreover, the in situ characterization of VC‐VO/HPC@S provides a rational inference for their phase evolution in the galvanostatic charge/discharge process. The formation of the V5S8 phase during electrochemical cycling primarily facilitates the interconversion of liquid‐phase polysulfides. Consequently, the VC‐VO/HPC@S cathodes exhibit excellent capacity performance (1484 mAh g−1 at 0.1 C) and ultrahigh cycle stability (0.045% decay rate per cycle at 5 C). The pouch cell exhibits a high energy density of 358 Wh kg−1. This approach explores the phase evolution of VC‐VO particles in an electrochemical environment and is valuable for the development of Li−S batteries with high area capacity and long cycle life.

Phase Evolution of VC‐VO Heterogeneous Particles to Facilitate Sulfur Species Conversion in Li−S Batteries

Most of the catalysts in lithium sulfur (Li-S) batteries present low electronic conductivity and the lithium polysulfides (LiPSs) must diffuse onto the surface of the carbon materials to achieve their conversion reaction. It is a significant challenge to achieve the instantaneous transformation of LiPSs to Li2 S in Li-S batteries to suppress the shuttle effect of LiPSs. Herein, a unique electron and ion co-conductive catalyst of carbon-coated Li1.4 Al0.4 Ti1.6 (PO4 )3 (C@LATP) is developed, which not only possesses strong adsorption to LiPSs, but, more importantly, also promotes the instantaneous conversion reaction of LiPSs to Li2 S. The C@LATP nanoparticles as catalytic active sites can synchronously and efficiently provide both Li ions and electrons to facilitate the conversion reaction of LiPSs. The conversion reaction path of LiPSs using C@LATP changes from traditional "adsorption-diffusion-conversion" to novel "adsorption-conversion," which effectively lowers the decomposition barrier of Li2 S6 and promotes faster conversion of LiPSs. The shuttle effect of LiPSs is considerably suppressed and utilization of sulfur is greatly improved. The Li-S batteries using C@LATP present excellent rate, cycling, and self-discharge properties. This work highlights the significance of electron and ion co-conductive solid-state electrolytes for the instantaneous transformation of LiPSs in advanced Li-S batteries.

Electron and Ion Co-Conductive Catalyst Achieving Instant Transformation of Lithium Polysulfide towards Li2S

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Electron and Ion Co-Conductive Catalyst Achieving Instant Transformation of Lithium Polysulfide towards Li2S