Commercial lithium-ion (Li-ion) batteries suffer from low energy density and do not meet the growing demands of the energy storage market. Therefore, building next-generation rechargeable Li and Li-ion batteries with higher energy densities, better safety characteristics, lower cost and longer cycle life is of outmost importance. To achieve smaller and lighter next-generation rechargeable Li and Li-ion batteries that can outperform commercial Li-ion batteries, several new energy storage chemistries are being extensively studied. In this review, we summarize the current trends and provide guidelines towards achieving this goal, by addressing batteries using high-voltage cathodes, metal fluoride electrodes, chalcogen electrodes, Li metal anodes, high-capacity anodes as well as useful electrolyte solutions. We discuss the choice of active materials, practically achievable energy densities and challenges faced by the respective battery systems. Furthermore, strategies to overcome remaining challenges for achieving energy characteristics are addressed in the hope of providing a useful and balanced assessment of current status and perspectives of rechargeable Li and Li-ion batteries.

Guidelines and trends for next-generation rechargeable lithium and lithium-ion batteries.

A review of lithium ion battery failure mechanisms and fire prevention strategies

Lithium–sulfur batteries (Li–S) have become a viable alternative to future energy storage devices. The electrochemical reaction based on lithium and sulfur promises an extraordinary theoretical energy density, which is far higher than current commercialized Li-ion batteries. However, the principal disadvantage impeding the success of Li–S batteries lies in the severe leakage and migration of soluble lithium polysulfide intermediates out of cathodes upon cycling. The loss of active sulfur species incurs significant capacity decay and poor battery lifespans. Considerable efforts have been devoted to developing various sulfur host materials that can effectively anchor lithium polysulfides. Herein, a comprehensive review is presented of recent advances in sulfur host materials. On the basis of the electrochemistry of Li–S batteries, the strategies for anchoring polysulfides are systematically categorized into physical confinement and chemical bonding. The structural merits of various sulfur host materials are highlighted, and the interaction mechanisms with sulfur species are discussed in detail, which provides valuable insights into the rational design and engineering of advanced sulfur host materials facilitating the commercialization of Li–S batteries. Future challenges and promising research prospects for sulfur host materials are proposed at the end of the review.

Host Materials Anchoring Polysulfides in Li–S Batteries Reviewed

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.

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

Despite the ever-growing demand in safe and high power/energy density of Li+ ion and Li metal rechargeable batteries (LIBs), materials-related challenges are responsible for the majority of performance degradation in such batteries. These challenges include electrochemically induced phase transformations, repeated volume expansion and stress concentrations at interfaces, poor electrical and mechanical properties, low ionic conductivity, dendritic growth of Li, oxygen release and transition metal dissolution of cathodes, polysulfide shuttling in Li-sulfur batteries, and poor reversibility of lithium peroxide/superoxide products in Li-O2 batteries. Owing to compelling physicochemical and structural properties, in recent years two-dimensional (2D) materials have emerged as promising candidates to address the challenges in LIBs. This Review highlights the cutting-edge advances of LIBs by using 2D materials as cathodes, anodes, separators, catalysts, current collectors, and electrolytes. It is shown that 2D materials can protect the electrode materials from pulverization, improve the synergy of Li+ ion deposition, facilitate Li+ ion flux through electrolyte and electrode/electrolyte interfaces, enhance thermal stability, block the lithium polysulfide species, and facilitate the formation/decomposition of Li-O2 discharge products. This work facilitates the design of safe Li batteries with high energy and power density by using 2D materials.

Two-Dimensional Materials to Address the Lithium Battery Challenges

High-performance lithium sulfur batteries enabled by a synergy between sulfur and carbon nanotubes

Sulfurized polyacrylonitrile (SPAN) is attractive as one of the most promising cathode candidates for commercial lithium–sulfur (Li–S) batteries due to its outstanding capacity reversibility and structural stability. However, the limited sulfur content of ∼40 wt% in the composite hinders its practical applications owing to insufficient areal/volumetric energy density, especially when used as flexible cathodes for wearable energy storage devices. Here, we report an ultrathin and condensed SPAN film synthesized via the in situ growth of ZIF-67 on electrospun fibers composed of PAN and CNTs, followed by a vulcanization process to generate surface-anchored CoS2 that effectively suppresses fiber swelling and film thickening. Simultaneously, conductive CoS2 helps expedite the redox kinetics of sulfur conversion for achieving high-performance Li–S cells with much improved areal capacity. This study refreshes current performance of SPAN cells with an ultrahigh initial areal capacity of 8.1 mA h cm−2 at a sulfur loading of up to 5.9 mg cm−2, as well as a superior capacity of 1322 mA h g−1 in the prototype pouch cell, demonstrating great prospects of the employed protocol for realizing flexible Li–S batteries with high energy density.

Anchoring MOF-derived CoS2 on sulfurized polyacrylonitrile nanofibers for high areal capacity lithium–sulfur batteries

The emerging market of wearable smart electronics calls for flexible energy storage solutions with high performance but low cost. To fulfill this demand, a novel method involving high-pressure and high-temperature filtration has been developed to fabricate flexible and freestanding thin-film electrodes with high packing density for lithium ion batteries. The method is universal, can be used for fabricating both cathodes and anodes, and is applicable for most electrochemically active materials. No organic solvent is involved throughout the fabrication process, demonstrating excellent environmental benignity. Despite of the absence of current collectors, electrochemical characterizations on a pair of proof-of-concept anode (graphite) and cathode (lithium iron phosphate) reveal good areal capacity and rate capability. Prototype full pouch cells constructed using the electrode pair demonstrate excellent deformability, durability, and power output, promising for practical implementation with low fabrication cost.

Freestanding Electrode Pairs with High Areal Density Fabricated under High Pressure and High Temperature for Flexible Lithium Ion Batteries

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High-performance lithium sulfur batteries enabled by a synergy between sulfur and carbon nanotubes

Anchoring MOF-derived CoS2 on sulfurized polyacrylonitrile nanofibers for high areal capacity lithium–sulfur batteries

Freestanding Electrode Pairs with High Areal Density Fabricated under High Pressure and High Temperature for Flexible Lithium Ion Batteries