Advances in the Development of Single‐Atom Catalysts for High‐Energy‐Density Lithium–Sulfur Batteries

Abstract

Although lithium-sulfur (Li-S) batteries are promising next-generation energy-storage systems, their practical applications are limited by the growth of Li dendrites and lithium polysulfide shuttling. These problems can be mitigated through the use of single-atom catalysts (SACs), which exhibit the advantages of maximal atom utilization efficiency (≈100%) and unique catalytic properties, thus effectively enhancing the performance of electrode materials in energy-storage devices. This review systematically summarizes the recent progress in SACs intended for use in Li-metal anodes, S cathodes, and separators, briefly introducing the operating principles of Li-S batteries, the action mechanisms of the corresponding SACs, and the fundamentals of SACs activity, and then comprehensively describes the main strategies for SACs synthesis. Subsequently, the applications of SACs and the principles of SACs operation in reinforced Li-S batteries as well as other metal-S batteries are individually illustrated, and the major challenges of SACs usage in Li-S batteries as well as future development directions are presented.

Single‐Atom‐Regulated Heterostructure of Binary Nanosheets to Enable Dendrite‐Free and Kinetics‐Enhanced Li–S Batteries

“…[14a,16] Typically, SACs-anchored TMCs/heterostructures are synthesized by methods such as high temperature migration/pyrolysis, impregnation/ion-exchange/coprecipitation, atomic layer deposition, and electrochemical reduction. [17] However, most of the existing methods are multi-step and difficult to achieve SACs loading while growing TMCs/heterostructure [18] and cannot completely prevent the aggregation of metal species into clusters and nanoparticles. This brings new challenges to the construction of ideal SACs to satisfy electrocatalytic and reaction kinetics enhancement demands in high-performance Li-S batteries.…”

MOF-derived MoP nanorods decorated with a N-doped thin carbon layer as a robust lithiophilic and sulfiphilic nanoreactor for high-performance Li–S batteries

“…With the development of human society and the worsening of environmental pollution, it has become urgent to establish a balance between meeting increasing energy demands and alleviating growing pressure on the environment. 1,2 Electricity can be directly obtained from clean energy sources, such as wind power, hydroelectric power, solar energy, etc., but these clean energy sources are all intermittent. Therefore, it is particularly indispensable to explore advanced energy storage and conversion devices with excellent performance.…”

“…12,13 These disadvantages will inevitably cause low levels of sulfur utilization and sluggish reaction kinetics, thereby resulting in unsatisfactory electrochemical performance. In the past few decades, great effort has been applied to overcome these issues, with the following main approaches: (1) the design and preparation of cathode materials with special structures; (2) conguring novel types of functional electrolytes; and (3) developing functional separators. 14,15 Among these, the rational design, preparation, and application of functional separators in batteries has been conrmed as an effective and convenient way to advance the performance and support the future practical application of Li-S batteries.…”

“…Catalysts derived from MOFs possess several merits which support their application in electrocatalysis: (i) metal-based nanoparticles generated during carbonization may be effective for electrocatalysis due to their combination of strong catalytic performance and good conductivity; 40,41 and (ii) MOF-derived products with a porous nature are benecial for mass transportation, hence contributing to the improvement of catalytic performance during electrocatalysis. 2,42 Among the available materials, TMPs derived from MOFs usually have high theoretical capacitance and excellent conductivity. These merits are attributed to the lower electronegativity of elemental P in phosphides compared with elemental O and C in the corresponding oxides and carbides, which can allow fast electronic transport and facilitate active redox reactions in the case of TMPs.…”

Combined physical confinement and chemical adsorption on co-doped hollow TiO2 for long-term cycle lithium–sulfur batteries

“…To tackle the daunting challenges, a diverse set of novel strategies have been exploited and introduced to regulate the transport and kinetic behaviors of lithium polysulfides, including physical containment, 6 chemical anchor, 7 and selective catalysis. 8 Those efforts have effectively improved the electrochemical stability of the sulfur electrode by the physical confinement of the nonpolar carbon nanomaterials and the chemical affinity/catalytic effect of the polar compounds. 9 Generally, the single strategy mentioned above can improve the “shuttle effect” of the sulfur electrode.…”