Lithium–sulfur (Li–S) batteries have attracted much attention in the field of electrochemical energy storage due to their high energy density and low cost. However, the “shuttle effect” of the sulfur cathode, resulting in poor cyclic performance, is a big barrier for the development of Li–S batteries. Herein, a novel sulfur cathode integrating sulfur, flexible carbon cloth, and metal–organic framework (MOF)‐derived N‐doped carbon nanoarrays with embedded CoP (CC@CoP/C) is designed. These unique flexible nanoarrays with embedded polar CoP nanoparticles not only offer enough voids for volume expansion to maintain the structural stability during the electrochemical process, but also promote the physical encapsulation and chemical entrapment of all sulfur species. Such designed CC@CoP/C cathodes with synergistic confinement (physical adsorption and chemical interactions) for soluble intermediate lithium polysulfides possess high sulfur loadings (as high as 4.17 mg cm–2) and exhibit large specific capacities at different C‐rates. Specially, an outstanding long‐term cycling performance can be reached. For example, an ultralow decay of 0.016% per cycle during the whole 600 cycles at a high current density of 2C is displayed. The current work provides a promising design strategy for high‐energy‐density Li–S batteries.

To solve the serious problems (the agglomeration of nano-Fe, dissolution of polysulfide, and low electronic conductivity of LiS) of earth-abundant pyrite (FeS) cathodes for lithium batteries, a simple in situ encapsulation and transformation route has been successfully developed to synthesis pitaya-structured porous carbon embedded with FeS nanoparticles. Due to such a hierarchical architecture design, this cathode of pitaya-structured FeS@C can effectively avoid the serious agglomeration and coarsening of small Fe nanoparticles, reduce the dissolution of polysulfide, and provide superior kinetics toward lithium storage, resulting in enhanced reversibility and rate capability. Cycling in the voltage region of 1.0-3.0 V at 0.3 A g, the current conversion-based FeS@C cathode displays a high and stable energy density (about 1100 Wh kg), ultrahigh rate capability (a reversible capability of 660, 609, 554, 499, 449, and 400 mA h g at 0.2, 0.5, 1.0, 2.0, 5.0, and 10 A g, respectively), and stable cycling performance.

For solving the drawbacks of low conductivity and the shuttle effect in a sulfur cathode, various nonpolar carbon and polar metal compounds with strong chemical absorption ability are applied as sulfur host materials for lithium–sulfur (Li–S) batteries. Nevertheless, previous research simply attributed the performance improvement of sulfur cathodes to the chemical adsorption ability of polar metal compounds toward lithium polysulfides (LPS), while a deep understanding of the enhanced electrochemical performance in these various sulfur hosts, especially at the molecular levels, is still unclear. Herein, for a mechanistic understanding of superior metal phosphide host in Li–S battery chemistry, an integrated phosphide-based host of CF/FeP@C (carbon cloth with grown FeP@C nanotube arrays) is chosen as the model, and this binder-free cathode can exclude interference from the binder and conductive additives. With a systematic electrochemical investigation of the loading sulfur in such oxide- and phosphide-based hosts (CF/Fe3O4@C and CF/FeP@C), it is found that CF/FeP@C@S shows much superior Li–S performances. The greatly enhanced performance of CF/FeP@C@S suggests that FeP can well suppress the shuttle effect of LPS and accelerate their transformation during the charge–discharge process. The first-principles calculations reveal the performance variations of Fe3O4 and FeP in Li–S batteries mainly because the shifts of the p band of the FeP could accelerate the interfacial electronics transfer dynamics by increasing the electronic concentration in the Fermi level of adsorbed Li2S4. The current work sheds light on the promising design of superior Li–S batteries from both theoretical and experimental aspects.

Conventional lithium-ion batteries, with flammable organic liquid electrolytes, have seriouss afety problems, which greatly limit their application.A ll-solid-state batteries (ASSBs) have received extensive attention from large-scale energy-storage fields,s uch as electric vehicles (EVs) and intelligent powerg rids, due to their benefits in safety,e nergy density,a nd thermostability.A st he key component of ASSBs, solid electrolytes determine the properties of ASSBs. In past decades, various kinds of solid electrolytes, such as polymers and inorganic electrolytes, have been explored.Amongt hese candidates, organic-inorganic composite solid electrolytes (CSEs) that integrate the advantages of these two differente lectrolytes have been regarded as promising electrolytes for high-performanceA SSBs, and extensive studies have been carried out. Herein,r ecent progress in organic-inorganic CSEs is summarized in terms of the inorganic component, electrochemical performance, effects of the inorganicc eramic nanostructure, and ionic conducting mechanism. Finally,t he main challenges and perspectiveso fo rganic-inorganic CSEs are highlighted for future development.

Solid‐state lithium metal batteries (SLMBs) are attracting enormous attention due to their enhanced safety and high theoretical energy density. However, the alkali lithium with high reducibility can react with the solid‐state electrolytes resulting in the inferior cycle lifespan. Herein, inspired by the idea of interface design, the 1‐butyl‐1‐methylpyrrolidinium bis(trifluoromethanesulfonyl) imide as an initiator to generate an artificial protective layer in polymer electrolyte is selected. Time‐of‐flight secondary ion mass spectrometry and X‐ray photoelectron spectroscopy reveal the stable solid electrolyte interface (SEI) is in situ formed between the electrolyte/Li interface. Scanning electron microscopy (SEM) images demonstrate that the constructed SEI can promote homogeneous Li deposition. As a result, the Li/Li symmetrical cells enable stable cycle ultralong‐term for over 4500 h. Moreover, the as‐prepared LiFePO 4 /Li SLMBs exhibit an impressive ultra‐long cycle lifespan over 1300 cycles at 1 C, as well as 1600 cycles at 0.5 C with a capacity retention ratio over 80%. This work offers an effective strategy for the construction of the stable electrolyte/Li interface, paving the way for the rapid development of long lifespan SLMBs.