Due to their high energy density and low material cost, lithium–sulfur batteries represent a promising energy storage system for a multitude of emerging applications, ranging from stationary grid storage to mobile electric vehicles. This review aims to summarize major developments in the field of lithium–sulfur batteries, starting from an overview of their electrochemistry, technical challenges and potential solutions, along with some theoretical calculation results to advance our understanding of the material interactions involved. Next, we examine the most extensively-used design strategy: encapsulation of sulfur cathodes in carbon host materials. Other emerging host materials, such as polymeric and inorganic materials, are discussed as well. This is followed by a survey of novel battery configurations, including the use of lithium sulfide cathodes and lithium polysulfide catholytes, as well as recent burgeoning efforts in the modification of separators and protection of lithium metal anodes. Finally, we conclude with an outlook section to offer some insight on the future directions and prospects of lithium–sulfur batteries.

Designing high-energy lithium–sulfur batteries

Amid burgeoning environmental concerns, electrochemical energy storage has rapidly gained momentum. Among the contenders in the ‘beyond lithium’ energy storage arena, the lithium–sulfur (Li–S) battery has emerged as particularly promising, owing to its potential to reversibly store considerable electrical energy at low cost. Whether or not Li–S energy storage will be able to fulfil this potential depends on simultaneously solving many aspects of its underlying conversion chemistry. Here, we review recent developments in tackling the dissolution of polysulfides — a fundamental problem in Li–S batteries — focusing on both experimental and computational approaches to tailor the chemical interactions between the sulfur host materials and polysulfides. We also discuss smart cathode architectures enabled by recent materials engineering, especially for high areal sulfur loading, as well as innovative electrolyte design to control the solubility of polysulfides. Key factors that allow long-life and high-loading Li–S batteries are summarized. Li–S batteries are a low-cost and high-energy storage system but their full potential is yet to be realized. This Review surveys recent advances in understanding polysulfide chemistry at the positive electrode and the electrolyte and discusses approaches towards long-life and high-loading batteries.

Advances in lithium-sulfur batteries based on multifunctional cathodes and electrolytes

Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable electronics, and to mitigate environmental problems. However, the application of Li–S batteries is challenged by several obstacles, including their short life and low sulfur utilization, which become more serious when sulfur loading is increased to the practically accepted level above 3–5 mg cm−2. More and more efforts have been made recently to overcome the barriers toward commercially viable Li–S batteries with a high sulfur loading. This review highlights the recent progress in high-sulfur-loading Li–S batteries enabled by hierarchical design principles at multiscale. Particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are under specific concerns. Hierarchy in the multiscale design is proposed to guide the future development of high-sulfur-loading Li–S batteries.

Review on High-Loading and High-Energy Lithium–Sulfur Batteries

Lithium-sulfur (Li-S) batteries have attracted tremendous interest because of their high theoretical energy density and cost effectiveness. The target of Li-S battery research is to produce batteries with a high useful energy density that at least outperforms state-of-the-art lithium-ion batteries. However, due to an intrinsic gap between fundamental research and practical applications, the outstanding electrochemical results obtained in most Li-S battery studies indeed correspond to low useful energy densities and are not really suitable for practical requirements. The Li-S battery is a complex device and its useful energy density is determined by a number of design parameters, most of which are often ignored, leading to the failure to meet commercial requirements. The purpose of this review is to discuss how to pave the way for reliable Li-S batteries. First, the current research status of Li-S batteries is briefly reviewed based on statistical information obtained from literature. This includes an analysis of how the various parameters influence the useful energy density and a summary of existing problems in the current Li-S battery research. Possible solutions and some concerns regarding the construction of reliable Li-S batteries are comprehensively discussed. Finally, insights are offered on the future directions and prospects in Li-S battery field.

More Reliable Lithium-Sulfur Batteries: Status, Solutions and Prospects.

Lithium-sulfur (Li-S) batteries with high energy density and long cycle life are considered to be one of the most promising next-generation energy-storage systems beyond routine lithium-ion batteries. Various approaches have been proposed to break down technical barriers in Li-S battery systems. The use of nanostructured metal oxides and sulfides for high sulfur utilization and long life span of Li-S batteries is reviewed here. The relationships between the intrinsic properties of metal oxide/sulfide hosts and electrochemical performances of Li-S batteries are discussed. Nanostructured metal oxides/sulfides hosts used in solid sulfur cathodes, separators/interlayers, lithium-metal-anode protection, and lithium polysulfides batteries are discussed respectively. Prospects for the future developments of Li-S batteries with nanostructured metal oxides/sulfides are also discussed.

Nanostructured Metal Oxides and Sulfides for Lithium-Sulfur Batteries

The lithium-sulfur battery is a compelling energy storage system because its high theoretical energy density exceeds Li-ion batteries at much lower cost, but applications are thwarted by capacity decay caused by the polysulfide shuttle. Here, proof of concept and the critical metrics of a strategy to entrap polysulfides within the sulfur cathode by their reaction to form a surface-bound active redox mediator are demonstrated. It is shown through a combination of surface spectroscopy and cyclic voltammetry studies that only materials with redox potentials in a targeted window react with polysulfides to form active surface-bound polythionate species. These species are directly correlated to superior Li-S cell performance by electrochemical studies of high surface area oxide cathodes with redox potentials below, above, and within this window. Optimized Li-S cells yield a very low fade rate of 0.048% per cycle. The insight gained into the fundamental surface mechanism and its correlation to the stability of the electrochemical cell provides a bridge between mechanistic understanding and battery performance essential for the design of high performance Li-S cells.

Tuning Transition Metal Oxide–Sulfur Interactions for Long Life Lithium Sulfur Batteries: The “Goldilocks” Principle

Rechargeable solid-state lithium ion batteries (SSLB) require fast ion conducting solid electrolytes (SEs) to enable high charge and discharge rates. Li7P3S11 is a particularly promising lithium solid electrolyte, exhibiting very high room temperature conductivities of up to 17 mS·cm–1 and high ductility, allowing fast ion transport through the bulk and intimate contact to high surface electrodes. Here we present a novel hot-press setup that facilitates the synthesis of solid electrolytes by combining in situ electrochemical impedance spectroscopy (EIS) with simultaneous temperature- and pressure-monitoring. While a high room temperature conductivity in the order of 10 mS·cm–1 is readily achieved for phase pure Li7P3S11 with this design, it further enables monitoring of the different steps of crystallization from an amorphous Li2S–P2S5 glass to triclinic Li7P3S11. Nucleation, crystallization and—at temperatures exceeding 280 °C—decomposition of the material are analyzed in real time, enabling process opti...

In Situ Monitoring of Fast Li-Ion Conductor Li7P3S11 Crystallization Inside a Hot-Press Setup

Lithium-Sulfur Batteries: Tuning Transition Metal Oxide–Sulfur Interactions for Long Life Lithium Sulfur Batteries: The “Goldilocks” Principle (Adv. Energy Mater. 6/2016)

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Tuning Transition Metal Oxide–Sulfur Interactions for Long Life Lithium Sulfur Batteries: The “Goldilocks” Principle

In Situ Monitoring of Fast Li-Ion Conductor Li7P3S11 Crystallization Inside a Hot-Press Setup

Lithium-Sulfur Batteries: Tuning Transition Metal Oxide–Sulfur Interactions for Long Life Lithium Sulfur Batteries: The “Goldilocks” Principle (Adv. Energy Mater. 6/2016)