Because of their high energy density, low cost, and environmental friendliness, lithium-sulfur (Li-S) batteries are one of the potential candidates for the next-generation energy-storage devices. However, they have been troubled by sluggish reaction kinetics for the insoluble Li2S product and capacity degradation because of the severe shuttle effect of polysulfides. These problems have been overcome by introducing transition metal compounds (TMCs) as catalysts into the interlayer of modified separator or sulfur host. This review first introduces the mechanism of sulfur redox reactions. The methods for studying TMC catalysts in Li-S batteries are provided. Then, the recent advances of TMCs (such as metal oxides, metal sulfides, metal selenides, metal nitrides, metal phosphides, metal carbides, metal borides, and heterostructures) as catalysts and some helpful design and modulation strategies in Li-S batteries are highlighted and summarized. At last, future opportunities toward TMC catalysts in Li-S batteries are presented.

Understanding the Catalytic Kinetics of Polysulfide Redox Reactions on Transition Metal Compounds in Li-S Batteries.

Lithium–sulfur batteries are one of the most promising alternatives for advanced battery systems due to the merits of extraordinary theoretical specific energy density, abundant resources, environmental friendliness, and high safety. However, the sluggish sulfur reduction reaction (SRR) kinetics results in poor sulfur utilization, which seriously hampers the electrochemical performance of Li–S batteries. It is critical to reveal the underlying reaction mechanisms and accelerate the SRR kinetics. Herein, the critical issues of SRR in Li–S batteries are reviewed. The conversion mechanisms and reaction pathways of sulfur reduction are initially introduced to give an overview of the SRR. Subsequently, recent advances in catalyst materials that can accelerate the SRR kinetics are summarized in detail, including carbon, metal compounds, metals, and single atoms. Besides, various characterization approaches for SRR are discussed, which can be divided into three categories: electrochemical measurements, spectroscopic techniques, and theoretical calculations. Finally, the conclusion and outlook part gives a summary and proposes several key points for future investigations on the mechanisms of the SRR and catalyst activities. This review can provide cutting‐edge insights into the SRR in Li–S batteries.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/aenm.202202094

Sulfur Reduction Reaction in Lithium–Sulfur Batteries: Mechanisms, Catalysts, and Characterization

The electrochemical performance of lithium‐sulfur (Li‐S) batteries is severely hindered by the sluggish sulfur redox kinetics and the shuttle effect of lithium polysulfides (LiPSs). Herein, an integrated composite catalyst consisting of Co nanoparticles and single‐atom (SA) Zn co‐implanted in nitrogen‐doped porous carbon nanosheets grafted with carbon nanotubes (Co/SA‐Zn@N‐C/CNTs) is rationally developed toward this challenge. Experimental and theoretical investigations indicate that the synergistically dual active sites of Co and atomic Zn‐N4 moieties with an optimal charge redistribution not only strongly confine the LiPSs but also effectively catalyze its conversion reactions by lowering the energy barrier from Li2S2 to Li2S while the N‐doped porous carbon‐grafted CNTs enables a large surface area for more active site exposure and provides a fast electron/ion pathway. Benefiting from synergies, Li‐S batteries equipped with the Co/SA‐Zn@N‐C/CNTs‐based sulfur cathode exhibit a high reversible capacity of 1302 mAh g−1 at 0.2 C and a low capacity fading rate of 0.033% per cycle over 800 cycles at 1 C. Moreover, a high areal capacity of 4.5 mAh cm−2 at 0.2 C with the sulfur loading of 5.1 mg cm−2 can be achieved. The present work may provide new insight into the design of high‐performance sulfur‐based cathodes for Li‐S batteries.

Implanting Single Zn Atoms Coupled with Metallic Co Nanoparticles into Porous Carbon Nanosheets Grafted with Carbon Nanotubes for High‐Performance Lithium‐Sulfur Batteries

Single-atom catalysts have been paid more attention to improving sluggish reaction kinetics and anchoring polysulfide for lithium-sulfur (Li-S) batteries. It has been demonstrated that d-block single-atom elements in the fourth period can chemically interact with the local environment, leading to effective adsorption and catalytic activity toward lithium polysulfides. Enlightened by theoretical screening, for the first time, we design novel single-atom Nb catalysts toward improved sulfur immobilization and catalyzation. Calculations reveal that Nb-N4 active moiety possesses abundant unfilled antibonding orbitals, which promotes d-p hybridization and enhances anchoring capability toward lithium polysulfides via a "trapping-coupling-conversion" mechanism. The Nb-SAs@NC cell exhibits a high capacity retention of over 85% after 1000 cycles, a superior rate performance of 740 mA h g-1 at 7 C, and a competitive areal capacity of 5.2 mAh cm-2 (5.6 mg cm-2). Our work provides a new perspective to extend cathodes enabling high-energy-density Li-S batteries.

d-p Hybridization-Induced "Trapping-Coupling-Conversion" Enables High-Efficiency Nb Single-Atom Catalysis for Li-S Batteries.

Aqueous zinc–ion batteries (ZIBs) have been promptly developed as a competitive and promising system for future large‐scale energy storage. In recent years, vanadium (V)‐based compounds, with diversity of valences and high electrochemical‐activity, have been widely studied as cathodes for aqueous ZIBs because of their rich reserves and high theoretical capacity. However, the stubborn issues including low conductivity and sluggish kinetics, plague their smooth application in aqueous ZIBs. Among various countermeasures, defect engineering is believed as an effective method to alleviate the above limitations. This review highlights the challenges of different V‐based cathode materials (e.g., vanadium oxides and vanadates) and summarizes the advances in defect engineering strategies including types and effects of the defects, designed strategies, and characterization techniques for high‐energy ZIBs. Finally, several sound prospects in this fervent field are also rationally proposed for fundamental research and practical application.

Advances on Defect Engineering of Vanadium‐Based Compounds for High‐Energy Aqueous Zinc–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

Witnessing compositional evolution and identifying the catalytically active moiety of electrocatalysts is of paramount importance in Li-S chemistry. Nevertheless, this field remains elusive. We report the scalable salt-templated synthesis of Se-vacancy-incorporated MoSe2 architecture (SeVs-MoSe2 ) and reveal the phase evolution of the defective precatalyst in working Li-S batteries. The interaction between lithium polysulfides and SeVs-MoSe2 is probed to induce the transformation from SeVs-MoSe2 to MoSeS. Furthermore, operando Raman spectroscopy and ex situ X-ray diffraction measurements in combination with theoretical simulations verify that the effectual MoSeS catalyst could help promote conversion of Li2 S2 to Li2 S, thereby boosting the capacity performance. The Li-S battery accordingly exhibits a satisfactory rate and cycling capability even with and elevated sulfur loading and lean electrolyte conditions (7.67 mg cm-2 ; 4.0 μL mg-1S ). This work elucidates the design strategies and catalytic mechanisms of efficient electrocatalysts bearing defects.

Identifying the Evolution of Selenium-Vacancy-Modulated MoSe2 Precatalyst in Lithium–Sulfur Chemistry

Identifying the Evolution of Se-Vacancy-Modulated MoSe2 Pre-Catalyst in Li–S Chemistry

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

Identifying the Evolution of Selenium-Vacancy-Modulated MoSe2 Precatalyst in Lithium–Sulfur Chemistry

Identifying the Evolution of Se-Vacancy-Modulated MoSe2 Pre-Catalyst in Li–S Chemistry