Lithium-ion batteries, which have revolutionized portable electronics over the past three decades, were eventually recognized with the 2019 Nobel Prize in chemistry. As the energy density of current lithium-ion batteries is approaching its limit, developing new battery technologies beyond lithium-ion chemistry is significant for next-generation high energy storage. Lithium-sulfur (Li-S) batteries, which rely on the reversible redox reactions between lithium and sulfur, appears to be a promising energy storage system to take over from the conventional lithium-ion batteries for next-generation energy storage owing to their overwhelming energy density compared to the existing lithium-ion batteries today. Over the past 60 years, especially the past decade, significant academic and commercial progress has been made on Li-S batteries. From the concept of the sulfur cathode first proposed in the 1960s to the current commercial Li-S batteries used in unmanned aircraft, the story of Li-S batteries is full of breakthroughs and back tracing steps. Herein, the development and advancement of Li-S batteries in terms of sulfur-based composite cathode design, separator modification, binder improvement, electrolyte optimization, and lithium metal protection is summarized. An outlook on the future directions and prospects for Li-S batteries is also offered.

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

Lithium-sulfur batteries are a major focus of academic and industrial energy-storage research due to their high theoretical energy density and the use of low-cost materials. The high energy density results from the conversion mechanism that lithium-sulfur cells utilize. The sulfur cathode, being naturally abundant and environmentally friendly, makes lithium-sulfur batteries a potential next-generation energy-storage technology. The current state of the research indicates that lithium-sulfur cells are now at the point of transitioning from laboratory-scale devices to a more practical energy-storage application. Based on similar electrochemical conversion reactions, the low-cost sulfur cathode can be coupled with a wide range of metallic anodes, such as sodium, potassium, magnesium, calcium, and aluminum. These new "metal-sulfur" systems exhibit great potential in either lowering the production cost or producing high energy density. Inspired by the rapid development of lithium-sulfur batteries and the prospect of metal-sulfur cells, here, over 450 research articles are summarized to analyze the research progress and explore the electrochemical characteristics, cell-assembly parameters, cell-testing conditions, and materials design. In addition to highlighting the current research progress, the possible future areas of research which are needed to bring conversion-type lithium-sulfur and other metal-sulfur batteries into the market are also discussed.

Current Status and Future Prospects of Metal–Sulfur Batteries

High-energy lithium metal batteries (LMBs) are expected to play important roles in the next-generation energy storage systems. However, the uncontrolled Li dendrite growth in liquid electrolytes still impedes LMBs from authentic commercialization. Upgrading the traditional electrolyte system from liquid to solid and quasi-solid has therefore become a key issue for prospective LMBs. From this premise, it is particularly urgent to exploit facile strategies to accomplish this goal. We report that commercialized liquid electrolyte can be easily converted into a novel quasi-solid gel polymer electrolyte (GPE) via a simple and efficient in situ gelation strategy, which, in essence, is to use LiPF6 to induce the cationic polymerization of the ether-based 1,3-dioxolane and 1,2-dimethoxyethane liquid electrolyte under ambient temperature. The newly developed GPE exhibits elevated protective effects on Li anodes and has universality for diversified cathodes including but not restricted to sulfur, olivine-type LiFePO4, and layered LiNi0.6Co0.2Mn0.2O2, revealing tremendous potential in promoting the large-scale application of future LMBs.

Upgrading traditional liquid electrolyte via in situ gelation for future lithium metal batteries.

Solid-state lithium–sulfur batteries (SSLSBs) with high energy densities and high safety have been considered among the most promising energy storage devices to meet the demanding market requirements for electric vehicles. However, critical challenges such as lithium polysulfide shuttling effects, mismatched interfaces, Li dendrite growth, and the gap between fundamental research and practical applications still hinder the commercialization of SSLSBs. This review aims to combine the fundamental and engineering perspectives to seek rational design parameters for practical SSLSBs. The working principles, constituent components, and practical challenges of SSLSBs are reviewed. Recent progress and approaches to understand the interfacial challenges via advanced characterization techniques and density functional theory (DFT) calculations are summarized and discussed. A series of design parameters including sulfur loading, electrolyte thickness, discharge capacity, discharge voltage, and cathode sulfur content are systematically analyzed to study their influence on the gravimetric and volumetric energy densities of SSLSB pouch cells. The advantages and disadvantages of recently reported SSLSBs are discussed, and potential strategies are provided to address the shortcomings. Finally, potential future directions and prospects in SSLSB engineering are examined.

Towards high-performance solid-state Li-S batteries: from fundamental understanding to engineering design.

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

Ultrahigh Phosphorus Doping of Carbon for High-Rate Sodium Ion Batteries Anode

Titanium disulfide (TiS2) is investigated as an advanced conversion electrode for sodium (Na)-ion batteries (NIB) in an ether-based electrolyte (NaPF6/glyme (DME)) The as-prepared TiS2 demonstrates a high reversible capacity of 1040 mA h g-1 at 02 A g-1 with the capacity contribution of 521 mA h g-1 in the voltage region below 10 V (vs Na/Na+), remarkable initial coulombic efficiency of 959% and superior rate capability of 621 mA h g-1 at 40 A g-1 The high conductivity of the Ti-based compounds and nanosized particles generated by chemical conversion reactions could minimize the entropic barrier for the reversible conversion, resulting in high reversibility and ultrafast charge/discharge ability of the electrode Moreover, with its strong ability to adsorb soluble polysulfide intermediates, the as-prepared TiS2 electrode exhibits superior cycling stability over 9000 cycles, serving as a stable and ultra-high capacity conversion electrode for NIBs

https://onlinelibrary.wiley.com/doi/pdf/10.1002/advs.201801021

TiS2 as an Advanced Conversion Electrode for Sodium-Ion Batteries with Ultra-High Capacity and Long-Cycle Life.

The permeation of dissolved lithium polysulfides across the porous polyolefin-based commercial separator is a major hindrance for using lithium sulfur batteries (LSBs). In this work, the poly(vinylidene fluoride) (PVDF)-based gel polymer electrolyte (GPE) with a compact morphology to block polysulfide penetration is prepared using a simple solution-casting method, and the strategy of incorporating poly(ethylene oxide) and nano zirconium dioxide is applied to guarantee electrolyte uptake and Li+ mobility. Superior to the commercial separator with liquid electrolyte, the LSB assembled with additive-free GPE exhibits a high initial capacity of 1429 mA h g−1, coulombic efficiency of 96% at 0.2C and improved rate performance. After 500 cycles at 1C, the LSB could still deliver a capacity of 847.2 mA h g−1, with a low fading rate of 0.05%. The LSB with high sulfur loading (5.2 mg cm−2) could attain a high areal capacity of 4.6 mA h cm−2. Results of scanning electron microscopy suggest that such a hybrid GPE could effectively protect the lithium anode from polysulfide corrosion. Therefore, this novel membrane of hybrid PVDF-based GPE provides a simple and effective method to establish high-performance LSBs.

Poly(vinylidene fluoride)-based hybrid gel polymer electrolytes for additive-free lithium sulfur batteries

Nanoengineering of metal electrodes are of great importance for improving the energy density of alkali-ion batteries, which have been deemed one of most effective tools for addressing the poor cycle stability of metallic anodes. However, the practical application of nanostructured electrodes in batteries is still challenged by a lack of efficient, low-cost, and scalable preparation methods. Herein, we propose a facile chemical dealloying approach to the tunable preparation of multidimensional Sb nanostructures. Depending on dealloying reaction kinetics regulated by different solvents, zero-dimensional Sb nanoparticles (Sb-NP), two-dimensional Sb nanosheets (Sb-NS), and three-dimensional nanoporous Sb are controllably prepared via etching Li-Sb alloys in H2O, H2O-EtOH, and EtOH, respectively. Morphological evolution mechanisms of the various Sb nanostructures are analyzed by scanning electron microscopy, transmission electron microscopy, and X-ray diffraction measurements. When applied as anodes for sodium ion batteries (SIBs), the as-prepared Sb-NS electrodes without any chemical modifications exhibit high reversible capacity of 620 mAh g-1 and retain 90.2% of capacity after 100 cycles at 100 mA g-1. The excellent Na+ storage performance observed is attributable to the two-dimensional nanostructure, which ensures high degrees of Na+ accessibility, robust structural integrity, and rapid electrode transport. This facile and tunable approach can broaden ways of developing high performance metal electrodes with designed nanostructures for electrochemical energy storage and conversion applications.

Facile Tailoring of Multidimensional Nanostructured Sb for Sodium Storage Applications.

A simple one-pot hydrothermal method is developed for fabrication of MoS2@rGO nanoflakes using the economical MoO3 as the molybdenum source. Benefiting from the unique nanoarchitecture, high MoS2 loading (90.3 wt%) and the expanded interlayer spacing, the as-prepared MoS2@rGO nanoflakes exhibit greatly enhanced sodium storage performances including a high reversible specific capacity of 441 mAh g−1 at a current density of 0.2 A g−1, high rate capability, and excellent capacity retention of 93.2% after 300 cycles.

/pdf/mos-2-rgo-nanoflakes-as-high-performance-anode-materials-in-xzv417rlk1.pdf

MoS 2 @rGO Nanoflakes as High Performance Anode Materials in Sodium Ion Batteries

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