Abstract
Benefiting from the merits of low cost, ultrahigh‐energy densities, and environmentally friendliness, metal–sulfur batteries (M–S batteries) have drawn massive attention recently. However, their practical utilization is impeded by the shuttle effect and slow redox process of polysulfide. To solve these problems, enormous creative approaches have been employed to engineer new electrocatalytic materials to relieve the shuttle effect and promote the catalytic kinetics of polysulfides. In this review, recent advances on designing principles and active centers for polysulfide catalytic materials are systematically summarized. At first, the currently reported chemistries and mechanisms for the catalytic conversion of polysulfides are presented in detail. Subsequently, the rational design of polysulfide catalytic materials from catalytic polymers and frameworks to active sites loaded carbons for polysulfide catalysis to accelerate the reaction kinetics is comprehensively discussed. Current breakthroughs are highlighted and directions to guide future primary challenges, perspectives, and innovations are identified. Computational methods serve an ever‐increasing part in pushing forward the active center design. In summary, a cutting‐edge understanding to engineer different polysulfide catalysts is provided, and both experimental and theoretical guidance for optimizing future M–S batteries and many related battery systems are offered.
Highlights
Benefiting from the merits of low cost, ultrahigh-energy densities, and electric vehicles and portable electronic devices, lithium-ion batteries (LIBs) gradually become insufficient to environmentally friendliness, metal–sulfur batteries (M–S batteries) have meet all the urgent demands on high energy drawn massive attention recently
This study indicated that S8 was relatively easy to convert to polysulfide, while the conversion of soluble polysulfide to insoluble reduction products showed slower kinetics by activation energy tests.[13]
The electric potential decreasing at the start of the second plateau derives from the concentration polarization due to the obstacle of Li+ conveyance by the enhancement of electrolyte viscosity,[3a,19] and the overpotential required by the crystallization of ionically/electrically insulating Li2S2.[20]. Low sulfur usage rate is caused by the inactive reaction kinetics in these steps
Summary
As for a Li–S battery, the sluggish charge transport and soluble polysulfides shuttling are always ascribed to the faint affinity between polysulfides and conventional carbon mediators. IV) The last ramp relates to the single-phase reaction from Li2S2 to Li2S.[18] The electric potential decreasing at the start of the second plateau derives from the concentration polarization due to the obstacle of Li+ conveyance by the enhancement of electrolyte viscosity,[3a,19] and the overpotential required by the crystallization of ionically/electrically insulating Li2S2.[20] Low sulfur usage rate is caused by the inactive reaction kinetics in these steps. To reduce the shuttle effect and improve the sulfur usage rate under high sulfur content, some reports showed that the rapid conversion between lithium polysulfide and Li2S2/Li2S on the active sites of the electrocatalytic materials is faster than on the polar adsorbents by the only adsorption. Them are beneficial to lower the reaction activation energy from soluble polysulfides to insoluble discharge products
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