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Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium–sulfur (Li‐S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li‐S pouch cells. Herein, we demonstrate that a rational combination of selenium doping, core–shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm−2) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm−2) with a low electrolyte/sulfur ratio (10 μL mg−1). This research further demonstrates a durable Li‐Se/S pouch cell with high specific capacity, validating the potential practical applications. [ABSTRACT FROM AUTHOR]

Berichtigung: Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries Keywords: cathodes; high-energy-density batteries; lithium metal anode; selenium-sulfur; solid-electrolyte interphase EN cathodes high-energy-density batteries lithium metal anode selenium-sulfur solid-electrolyte interphase 22278 22278 1 09/29/21 20211004 NES 211004 In this Research Article, Figure 2 and Figure 3 were swapped during the publication process. Cathodes, high-energy-density batteries, lithium metal anode, selenium-sulfur, solid-electrolyte interphase. [Extracted from the article]

Solid-electrolyte interphase, cathodes, high-energy-density batteries, lithium metal anode, selenium-sulfur Corrigendum: Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries Keywords: cathodes; high-energy-density batteries; lithium metal anode; selenium-sulfur; solid-electrolyte interphase EN cathodes high-energy-density batteries lithium metal anode selenium-sulfur solid-electrolyte interphase 22106 22106 1 09/29/21 20211004 NES 211004 In this Research Article, Figure 2 and Figure 3 were swapped during the publication process. [Extracted from the article]

Lithium/selenium‐sulfur batteries have recently received considerable attention due to their relatively high specific capacities and high electronic conductivity. Different from the traditional encapsulation strategy for suppressing the shuttle effect, an alternative approach to directly bypass polysulfide/polyselenide formation via rational solid‐electrolyte interphase (SEI) design is demonstrated. It is found that the robust SEI layer that in situ forms during charge/discharge via interplay between rational cathode design and optimal electrolytes could enable solid‐state (de)lithiation chemistry for selenium‐sulfur cathodes. Hence, Se‐doped S22.2Se/Ketjenblack cathodes can attain a high reversible capacity with minimal shuttle effects during long‐term and high rate cycling. Moreover, the underlying solid‐state (de)lithiation mechanism, as evidenced by in situ 7Li NMR and in operando synchrotron X‐ray probes, further extends the optimal sulfur confinement pore size to large mesopores and even macropores that have been long considered as inferior sulfur or selenium host materials, which play a crucial role in developing high volumetric energy density batteries. It is expected that the findings in this study will ignite more efforts to tailor the compositional/structure characteristics of the SEI layers and the related ionic transport across the interface by electrode structure, electrolyte solvent, and electrolyte additive screening. A solid‐electrolyte interphase resulting from rational cathode design and optimal electrolytes enables solid‐state lithiation chemistry for Li/S and Li/Se‐S batteries, which can directly bypass the formation of highly soluble polysulfides/polyselenides, and hence significantly improve shuttle effects and long‐term cycle stability. [ABSTRACT FROM AUTHOR]