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All‐solid‐state lithium batteries have emerged as a priority candidate for the next generation of safe and energy‐dense energy storage devices surpassing state‐of‐art lithium‐ion batteries. Among multitudinous solid‐state batteries based on solid electrolytes (SEs), sulfide SEs have attracted burgeoning scrutiny due to their superior ionic conductivity and outstanding formability. However, from the perspective of their practical applications concerning cell integration and production, it is still extremely challenging to constructing compatible electrolyte/electrode interfaces and developing available scale processing technologies. This review presents a critical overview of the current underlying understanding of interfacial issues and analyzes the main processing challenges faced by sulfide‐based all‐solid‐state batteries from the aspects of cost‐effective and energy‐dense design. Besides, the corresponding approaches involving interface engineering and processing protocols for addressing these issues and challenges are summarized. Fundamental and engineering perspectives on future development avenues toward practical application of high energy, safety, and long‐life sulfide‐based all‐solid‐state batteries are ultimately provided. Sulfide‐based all‐solid‐state lithium batteries have emerged as a priority candidate for the next generation of energy‐dense and safe energy storage devices. This review presents a critical overview of the current underlying understanding of interfacial issues and analyzes the main processing challenges faced by sulfide‐based all‐solid‐state batteries. The corresponding approaches involving interface engineering and processing protocols are highlighted. Fundamental and engineering perspectives on future development avenues toward their practical application are also presented.

Silicon (Si)‐based solid‐state batteries (Si‐SSBs) are attracting tremendous attention because of their high energy density and unprecedented safety, making them become promising candidates for next‐generation energy storage systems. Nevertheless, the commercialization of Si‐SSBs is significantly impeded by enormous challenges including large volume variation, severe interfacial problems, elusive fundamental mechanisms, and unsatisfied electrochemical performance. Besides, some unknown electrochemical processes in Si‐based anode, solid‐state electrolytes (SSEs), and Si‐based anode/SSE interfaces are still needed to be explored, while an in‐depth understanding of solid–solid interfacial chemistry is insufficient in Si‐SSBs. This review aims to summarize the current scientific and technological advances and insights into tackling challenges to promote the deployment of Si‐SSBs. First, the differences between various conventional liquid electrolyte‐dominated Si‐based lithium‐ion batteries (LIBs) with Si‐SSBs are discussed. Subsequently, the interfacial mechanical contact model, chemical reaction properties, and charge transfer kinetics (mechanical–chemical kinetics) between Si‐based anode and three different SSEs (inorganic (oxides) SSEs, organic–inorganic composite SSEs, and inorganic (sulfides) SSEs) are systemically reviewed, respectively. Moreover, the progress for promising inorganic (sulfides) SSE‐based Si‐SSBs on the aspects of electrode constitution, three‐dimensional structured electrodes, and external stack pressure is highlighted, respectively. Finally, future research directions and prospects in the development of Si‐SSBs are proposed. This review provides a systematic overview of silicon‐based solid‐state batteries (Si‐SSBs), focusing on the different interfacial configuration characteristics and mechanisms between various types of solid‐state electrolytes and Si‐based anodes as well as the correlations between these interfacial characteristics and electrochemical performance. We envision that this review can point navigation for benefiting the future advancement of Si‐SSBs.

Solid polymer electrolytes are light-weight, flexible, and non-flammable and provide a feasible solution to the safety issues facing lithium-ion batteries through the replacement of organic liquid electrolytes. Substantial research efforts have been devoted to achieving the next generation of solid-state polymer lithium batteries. Herein, we provide a review of the development of solid polymer electrolytes and provide comprehensive insights into emerging developments. In particular, we discuss the different molecular structures of the solid polymer matrices, including polyether, polyester, polyacrylonitrile, and polysiloxane, and their interfacial compatibility with lithium, as well as the factors that govern the properties of the polymer electrolytes. The discussion aims to give perspective to allow the strategic design of state-of-the-art solid polymer electrolytes, and we hope it will provide clear guidance for the exploration of high-performance lithium batteries.

Coupling electrochemical CO2 reduction (CO2R) with a renewable energy source to create high‐value fuels and chemicals is a promising strategy in moving toward a sustainable global energy economy. CO2R liquid products, such as formate, acetate, ethanol, and propanol, offer high volumetric energy density and are more easily stored and transported than their gaseous counterparts. However, a significant amount (~30%) of  liquid products from electrochemical CO2R in a flow cell reactor cross the ion exchange membrane, leading to the substantial loss of system‐level Faradaic efficiency. This severe crossover of the liquid product has—until now—received limited attention. Here, we review promising methods to suppress liquid product crossover, including the use of bipolar membranes, solid‐state electrolytes, and cation‐exchange membranes‐based acidic CO2R systems. We then outline the remaining challenges and future prospects for the production of concentrated liquid products from CO2. Here we review promising methods to suppress liquid product crossover in flow cell reactor including the use of bipolar membranes, solid‐state electrolytes, and cation‐exchange membranes based acidic CO2R systems. The elimination of liquid product crossover is thus a key step to advance the achievement of renewable liquid fuels from CO2

Highlights The lithium-ion conduction mechanism of organic-inorganic composite solid electrolytes (OICSEs) is thoroughly conducted and concluded from the microscopic perspective based on filler content, type, and system. The classic inorganic filler types, including inert and active fillers, are categorized with special emphasis on the relationship between inorganic filler structure design and the electrochemical performance of OICSEs. Advanced characterization techniques for OICSEs are discussed, and the challenges and prospects for developing superior all-solid-state lithium batteries are highlighted. To address the limitations of contemporary lithium-ion batteries, particularly their low energy density and safety concerns, all-solid-state lithium batteries equipped with solid-state electrolytes have been identified as an up-and-coming alternative. Among the various SEs, organic–inorganic composite solid electrolytes (OICSEs) that combine the advantages of both polymer and inorganic materials demonstrate promising potential for large-scale applications. However, OICSEs still face many challenges in practical applications, such as low ionic conductivity and poor interfacial stability, which severely limit their applications. This review provides a comprehensive overview of recent research advancements in OICSEs. Specifically, the influence of inorganic fillers on the main functional parameters of OICSEs, including ionic conductivity, Li + transfer number, mechanical strength, electrochemical stability, electronic conductivity, and thermal stability are systematically discussed. The lithium-ion conduction mechanism of OICSE is thoroughly analyzed and concluded from the microscopic perspective. Besides, the classic inorganic filler types, including both inert and active fillers, are categorized with special emphasis on the relationship between inorganic filler structure design and the electrochemical performance of OICSEs. Finally, the advanced characterization techniques relevant to OICSEs are summarized, and the challenges and perspectives on the future development of OICSEs are also highlighted for constructing superior ASSLBs.

HighlightsThe design, preparation and application of poly(ethylene oxide) (PEO)/ceramic composite solid electrolytes (CSEs) are summarized from “ceramic in polymer” and “polymer in ceramic”.The summary and outlook on existing challenges and future research directions of PEO/ceramic CSEs for lithium metal batteries are proposed.Composite solid electrolytes (CSEs) with poly(ethylene oxide) (PEO) have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li+ solvating capability, flexible processability and low cost. However, unsatisfactory room-temperature ionic conductivity, weak interfacial compatibility and uncontrollable Li dendrite growth seriously hinder their progress. Enormous efforts have been devoted to combining PEO with ceramics either as fillers or major matrix with the rational design of two-phase architecture, spatial distribution and content, which is anticipated to hold the key to increasing ionic conductivity and resolving interfacial compatibility within CSEs and between CSEs/electrodes. Unfortunately, a comprehensive review exclusively discussing the design, preparation and application of PEO/ceramic-based CSEs is largely lacking, in spite of tremendous reviews dealing with a broad spectrum of polymers and ceramics. Consequently, this review targets recent advances in PEO/ceramic-based CSEs, starting with a brief introduction, followed by their ionic conduction mechanism, preparation methods, and then an emphasis on resolving ionic conductivity and interfacial compatibility. Afterward, their applications in solid-state lithium metal batteries with transition metal oxides and sulfur cathodes are summarized. Finally, a summary and outlook on existing challenges and future research directions are proposed.

This review article deals with the ionic conductivity of solid‐state electrolytes for lithium batteries. It has discussed the mechanisms of ion conduction in ceramics, polymers, and ceramic‐polymer composite electrolytes. In ceramic electrolytes, ion transport is accomplished with mobile point defects in a crystal. Li+ ions migrate mainly via the vacancy mechanism, interstitial mechanism, or interstitial‐substitutional exchange mechanism. In solid polymer electrolytes, Li+ ions are transported mainly via the segment motion, ion hopping (Grotthuss mechanism), or vehicle mechanism (mass diffusion). This study has also introduced various electrolyte materials including perovskite oxides, garnet oxides, sodium superionic conductors, phosphates, sulfides, halides, cross‐linked polymers, block‐copolymers, metal‐organic frameworks, covalent organic frameworks, as well as ceramic‐polymer composites. In addition, it has highlighted some strategies to improve the ionic conductivity of solid‐state electrolytes, such as doping, defect engineering, microstructure tuning, and interface modification. This study gives a comprehensive review of the ionic conductivity of solid‐state electrolytes for lithium batteries. It discusses the mechanisms of ion conduction in ceramics, polymers, and ceramic‐polymer composite electrolytes, and highlights some strategies to improve the ionic conductivity of solid‐state electrolytes.

Traditional lithium–air batteries (LABs) have been seriously affected by cycle performance and safety issues due to many problems such as the volatility and leakage of liquid organic electrolyte, the generation of interface byproducts, and short circuits caused by the penetration of anode lithium dendrite, which has hindered its commercial application and development. In recent years, the emergence of solid-state electrolytes (SSEs) for LABs well alleviated the above problems. SSEs can prevent moisture, oxygen, and other contaminants from reaching the lithium metal anode, and their inherent performance can solve the generation of lithium dendrites, making them potential candidates for the development of high energy density and safety LABs. This paper mainly reviews the research progress of SSEs for LABs, the challenges and opportunities for synthesis and characterization, and future strategies are addressed.

Among the promising batteries for electric vehicles, rechargeable Li‐air (O2) batteries (LABs) have risen keen interest due to their high energy density. However, safety issues of conventional nonaqueous electrolytes remain the bottleneck of practical implementation of LABs. Solid‐state electrolytes (SSEs) with non‐flammable and eco‐friendly properties are expected to alleviate their safety concerns, which have become a research focus in the research field of LABs. Herein, we present a systematic review on the progress of SSEs for rechargeable LABs, mainly focusing on the interfacial issues existing between the SSEs and electrodes. The discussion highlights the challenges and feasible strategies for designing suitable SSEs for LABs. Solid‐state electrolytes with non‐flammable and eco‐friendly properties are expected to alleviate their safety concerns, which have become a research focus in the research field of Li‐air batteries (LABs). Herein, an overview of the recent progress in SSE‐based LAB (SSLABs) by categories of gel polymer electrolyte, solid polymer electrolyte, solid inorganic electrolyte, and solid composite electrolyte based batteries and the remaining interfacial challenges and possible solutions for the further development of SSLABs.

HighlightsThe poly(1,3-dioxolane) (PDOL) electrolyte demonstrates promising potential for practical application due to its advantages in in-situ polymerization process, high ionic conductivity, and long cycle life.This review focuses on the polymerization mechanism, composite innovation, and application of PDOL electrolytes.This review provides a comprehensive summary of the challenges associated with the PDOL electrolyte and makes forward-looking recommendations.Polymer solid-state lithium batteries (SSLB) are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety. Ion conductivity, interface stability and battery assembly process are still the main challenges to hurdle the commercialization of SSLB. As the main component of SSLB, poly(1,3-dioxolane) (PDOL)-based solid polymer electrolytes polymerized in-situ are becoming a promising candidate solid electrolyte, for their high ion conductivity at room temperature, good battery electrochemical performances, and simple assembly process. This review analyzes opportunities and challenges of PDOL electrolytes toward practical application for polymer SSLB. The focuses include exploring the polymerization mechanism of DOL, the performance of PDOL composite electrolytes, and the application of PDOL. Furthermore, we provide a perspective on future research directions that need to be emphasized for commercialization of PDOL-based electrolytes in SSLB. The exploration of these schemes facilitates a comprehensive and profound understanding of PDOL-based polymer electrolyte and provides new research ideas to boost them toward practical application in solid-state batteries.