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.

A novel cable-type flexible supercapacitor with excellent performance is fabricated using 3D polypyrrole(PPy)-MnO2 -CNT-cotton thread multi-grade nanostructure-based electrodes. The multiple supercapacitors with a high areal capacitance 1.49 F cm(-2) at a scan rate of 1 mV s(-1) connected in series and in parallel can successfully drive a LED segment display. Such an excellent performance is attributed to the cumulative effect of conducting single-walled carbon nanotubes on cotton thread, active mesoporous flower-like MnO2 nanoplates, and PPy conductive wrapping layer improving the conductivity, and acting as pseudocapacitance material simultaneously.

Cable-type supercapacitors of three-dimensional cotton thread based multi-grade nanostructures for wearable energy storage

The ever-increasing demand for flexible and portable electronics has stimulated research and development in building advanced electrochemical energy devices which are lightweight, ultrathin, small in size, bendable, foldable, knittable, wearable, and/or stretchable. In such flexible and portable devices, semi-solid/solid electrolytes besides anodes and cathodes are the necessary components determining the energy/power performances. By serving as the ion transport channels, such semi-solid/solid electrolytes may be beneficial to resolving the issues of leakage, electrode corrosion, and metal electrode dendrite growth. In this paper, the fundamentals of semi-solid/solid electrolytes (e.g., chemical composition, ionic conductivity, electrochemical window, mechanical strength, thermal stability, and other attractive features), the electrode-electrolyte interfacial properties, and their relationships with the performance of various energy devices (e.g., supercapacitors, secondary ion batteries, metal-sulfur batteries, and metal-air batteries) are comprehensively reviewed in terms of materials synthesis and/or characterization, functional mechanisms, and device assembling for performance validation. The most recent advancements in improving the performance of electrochemical energy devices are summarized with focuses on analyzing the existing technical challenges (e.g., solid electrolyte interphase formation, metal electrode dendrite growth, polysulfide shuttle issue, electrolyte instability in half-open battery structure) and the strategies for overcoming these challenges through modification of semi-solid/solid electrolyte materials. Several possible directions for future research and development are proposed for going beyond existing technological bottlenecks and achieving desirable flexible and portable electrochemical energy devices to fulfill their practical applications. It is expected that this review may provide the readers with a comprehensive cross-technology understanding of the semi-solid/solid electrolytes for facilitating their current and future researches on the flexible and portable electrochemical energy devices.

Opportunities of Flexible and Portable Electrochemical Devices for Energy Storage: Expanding the Spotlight onto Semi-solid/Solid Electrolytes.

Novel flexible storage devices such as supercapacitors and rechargeable batteries are of great interest due to their broad potential applications in flexible electronics and implants. Hydrogels are crosslinked hydrophilic polymer networks filled with water, and considered one of the most promising electrolyte candidates due to their high-water absorbency and softness that fulfilled the fundamental requirements for flexible energy storage devices. Moreover, diverse properties such as self-healing ability, ultra-stretchability, electrochromism, and extreme-temperature resistance can be achieved by modifying the chemical structures, opening the door to the development of novel flexible energy storage devices with prolonged service life and scintillating functions. In this review, we discuss the design methods of recent hydrogel electrolytes for supercapacitors and batteries regarding their electrochemical performance and highlight those with exceptional breakthrough and additional functions. Finally, challenges and prospects of future development are explored.

Recent advances of hydrogel electrolytes in flexible energy storage devices

Research progress on gel polymer electrolytes for lithium-sulfur batteries

The shuttle of the long-chain lithium polysulfides (LiPSs) is the main obstacle to the practical application of lithium-sulfur batteries. Herein, a poly(butyl acrylate/1-ethyl-3-vinylimidazole bis[(trifluoromethyl)sulfonyl]imide)-based quasi-solid-state copolymer electrolyte poly(ethylene glycol) diacrylate (PEGDA-P(BA-co-[EVIm]TFSI) QPE-IL) was prepared for lithium-sulfur batteries. The butyl acrylate component with abundant ester groups ensures the strong chemical capture for LiPSs. What is more, the introduction of ionic liquid ([EVIm]TFSI) can greatly improve the ionic conductivity and lithium-ion migration rate. More importantly, the dynamic-reversible adsorption of LiPSs was realized by chemical adsorption of ester-rich groups and electrostatic repulsion of free-moving negatively charged ions. As a result, the lithium-sulfur battery assembled by a reduced graphene oxide/carbon nanotube film@sulfur (rGOCTF@S) self-supporting cathode and QPE-IL displayed a high initial discharge capacity of 1179 mA h g-1, good cycling stability (72% capacity retention after 200 cycles at 0.5 C), and superior rate performance.

Poly(ionic liquid)-Based Quasi-Solid-State Copolymer Electrolytes for Dynamic-Reversible Adsorption of Lithium Polysulfides in Lithium-Sulfur Batteries.

A novel poly(vinyl carbonate-co-butyl acrylate) quasi-solid-state electrolyte as a strong catcher for lithium polysulfide in Li–S batteries

Solid-state polymer electrolytes are expected to fundamentally solve the instability and safety problems of liquid electrolytes for lithium–sulfur batteries. Herein, ionic liquids were introduced on the basis of constructing ester-rich copolymers, and dual Li-ion migration channels were built in an ester-rich copolymer/ionic liquid quasi-solid-state electrolyte (SPE-IL). “Association–disassociation” with the carbonyl groups and rapid ion exchange with the ionic liquids are the two migration modes that synergistically increase the room temperature ionic conductivity of the SPE-IL. In addition, the abundant ester groups provide strong chemisorption on lithium polysulfides and successfully inhibit the sulfur shuttle. More importantly, ionic liquids realize the “soft contact” between the electrode and the electrolyte, which is conducive to the construction of stable interfaces. Together with the GPa-level high modulus brought by vinyl carbonate, the formation of lithium dendrites is inhibited. As a result, the assembled lithium–sulfur battery displayed a high initial discharge capacity of 1106 mA h g−1, good cycling stability (80.2% capacity retention after 300 cycles at 0.1 C) and superior rate performance.

Dual Li-ion migration channels in an ester-rich copolymer/ionic liquid quasi-solid-state electrolyte for high-performance Li–S batteries

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Poly(ionic liquid)-Based Quasi-Solid-State Copolymer Electrolytes for Dynamic-Reversible Adsorption of Lithium Polysulfides in Lithium-Sulfur Batteries.

A novel poly(vinyl carbonate-co-butyl acrylate) quasi-solid-state electrolyte as a strong catcher for lithium polysulfide in Li–S batteries

Dual Li-ion migration channels in an ester-rich copolymer/ionic liquid quasi-solid-state electrolyte for high-performance Li–S batteries