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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.

The use of metal–organic frameworks (MOFs) in solid‐state electrolytes (SSEs) has been a very attractive research area that has received widespread attention in the modern world. SSEs can be divided into different types, some of which can be combined with MOFs to improve the electrochemical performance of the batteries by taking advantage of the high surface area and high porosity of MOFs. However, it also faces many serious problems and challenges. In this review, different types of SSEs are classified and the changes in these electrolytes after the addition of MOFs are described. Afterward, these SSEs with MOFs attached are introduced for different types of battery applications and the effects of these SSEs combined with MOFs on the electrochemical performance of the cells are described. Finally, some challenges faced by MOFs materials in batteries applications are presented, then some solutions to the problems and development expectations of MOFs are given. The use of metal–organic frameworks (MOFs) in solid‐state electrolytes (SSEs) has received widespread attention in the modern world. SSEs can be divided into different types, some of which can be combined with MOFs to improve the electrochemical performance of the battery by taking advantage of the high surface area and high porosity of MOFs.

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

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.

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.

Solid‐state electrolytes are critical for the development of next‐generation high‐energy and high‐safety rechargeable batteries. Among all the candidates, sodium (Na) superionic conductors (NASICONs) are highly promising because of their evident advantages in high ionic conductivity and high chemical/electrochemical stability. The concept of NASICONs was proposed by Hong and Goodenough et al. in 1976 by reporting the synthesis and characterization of Na1+xZr2(SixP3−x)O12 (0 ≤ x ≤ 3), which has attracted tremendous attention on the NASICONs‐type solid‐state electrolytes. In this review, we are committed to describing the development history of NASICONs‐type solid‐state electrolytes and elucidating the contribution of Goodenough as a tribute to him. We summarize the correlations and differences between lithium‐based and sodium‐based NASICONs electrolytes, such as their preparation methods, structures, ionic conductivities, and the mechanisms of ion transportation. Critical challenges of NASICONs‐structured electrolytes are discussed, and several research directions are proposed to tackle the obstacles toward practical applications. Sodium superionic conductors (NASICONs) with a three‐dimensional framework exhibit high ionic conductivity and stability under air and are a promising candidate for the solid‐state electrolyte. This review illustrates the history, physiochemical properties, challenges, and addresses solutions for NASICONs to guide future research.

Potassium (K)‐based batteries are viewed as the most promising alternatives to lithium‐based batteries, owing to their abundant potassium resource, lower redox potentials (−2.97 V vs. SHE), and low cost. Recently, significant achievements on electrode materials have boosted the development of potassium‐based batteries. However, the poor interfacial compatibility between electrode and electrolyte hinders their practical. Hence, rational design of electrolyte/electrode interface by electrolytes is the key to develop K‐based batteries. In this review, the principles for formulating organic electrolytes are comprehensively summarized. Then, recent progress of various liquid organic and solid‐state K+ electrolytes for potassium‐ion batteries and beyond are discussed. Finally, we offer the current challenges that need to be addressed for advanced K‐based batteries. This review mainly focuses on the recent progress of various liquid organic and solid‐state K+ electrolytes for potassium‐based batteries. First, the key design principles and applications of organic liquid electrolyte in various battery systems are discussed. Then the research status of ionic liquid, gel/polymer, and solid electrolyte are summarized and evaluated. Finally, this review discusses the challenge of various electrolyte/electrode interfaces and puts forward promising research direction and opportunities in the future.

All‐solid‐state lithium (Li) metal batteries combine high power density with robust security, making them one of the strong competitors for the next generation of battery technology. By replacing the flammable and volatile electrolytes commonly found in traditional Li‐ion batteries (LIBs) with noncombustible solid‐state electrolytes (SSEs), we have the potential to fundamentally enhance safety measures. Concurrently, SSE would be capable of fitting high specific capacity (3860 mAh g−1) metal Li and is expected to break through the upper limit of mass‐energy density (350 Wh kg−1) of existing LIBs system. Nevertheless, the growth of Li dendrites on the negative side or the nucleation of Li inside SSEs may give rise to battery short circuits, which is the primary factor limiting the application of Li metal. Recognizing this, the focus of this review is to provide a perspective for experimentalists and theorists who closely monitor various surface/interface and microstructure phenomena to understand Li dendrites. The strategies to reveal the complicated deposition mechanism and to control the dendrite growth of metal Li in solid‐state batteries, as well as the advanced characterization methods of metal Li, provide suggestions for the practical research of solid‐state Li metal batteries. All‐solid‐state batteries have attracted great attention from academia and industry, however, many challenges remain regarding practical applications. This review focuses on systematic discussions classifying the deposition mechanism of lithium (Li) dendrites, examining the ion concentration gradient, morphological characteristics of dendrites, and the nonuniform distribution of internal compressive stress, in the mainstream of solid‐state electrolytes. It delves into strategies for controlling Li metal deposition within the solid‐state electrolyte, compiles characterization methods for assessing Li deposition behavior in solid‐state batteries, and outlines anode design methodologies for industrialization. The review aims to offer some insights into the advancement of solid‐state batteries.

Li1.3Al0.3Ti1.7(PO4)3 (LATP) is one of the most attractive solid‐state electrolytes (SSEs) for application in all‐solid‐state lithium batteries (ASSLBs) due to its advantages of high ionic conductivity, air stability and low cost. However, the poor interfacial contact and slow Li‐ion migration have greatly limited its practical application. Herein, a composite ion‐conducting layer is designed at the Li/LATP interface, which a MoS2 film is constructed on LATP via chemical vapor deposition, followed by the introduction of a solid polymer (SP) liquid precursor to form a MoS2@SP protective layer. This protective layer not only achieves a lower Li‐ion migration energy barrier, but also adsorbs more Li‐ion, which is able to promote interfacial ion transport and improve interfacial contacts. Thanks to the improved migration and adsorption of Li‐ion, the Li symmetric cell containing LATP‐MoS2@SP exhibits a stable cycle of more than 1200 h at 0.1 mA cm−2. More remarkably, the capacity retention of the full cell assembled with LiFePO4 cathode is as high as 86.2% after 400 cycles at 1 C. This work provides a design strategy for significantly improving unstable interfaces of SSEs and realizing high‐performance ASSLBs. A composite ion‐conducting protective layer of MoS2/solid polymer is designed onto Li1.3Al0.3Ti1.7(PO4)3 (LATP), improving its poor Li/LATP interfacial contact and slow Li‐ion migration issues, which obtains excellent electrochemical performance. This study emphasizes the importance of promoting ion migration and adsorption in improving the interface, confirmed by density functional theory calculations and a series of experimental characterizations.

Halide solid‐state electrolytes (SSEs) hold promise for the commercialization of all‐solid‐state lithium batteries (ASSLBs); however, the currently cost‐effective zirconium‐based chloride SSEs suffer from hygroscopic irreversibility, low ionic conductivity, and inadequate thermal stability. Herein, a novel indium‐doped zirconium‐based chloride is fabricated to satisfy the abovementioned requirements, achieving outstanding‐performance ASSLBs at room temperature. Compared to the conventional Li2ZrCl6 and Li3InCl6 SSEs, the hc‐Li2+xZr1‐xInxCl6 (0.3 ≤ x ≤ 1) possesses higher ionic conductivity (up to 1.4 mS cm−1), and thermal stability (350 °C). At the same time, the hc‐Li2.8Zr0.2In0.8Cl6 also shows obvious hygroscopic reversibility, where its recovery rate of the ionic conductivity is up to 82.5% after 24‐h exposure in the 5% relative humidity followed by heat treatment. Theoretical calculation and experimental results reveal that those advantages are derived from the lattice expansion and the formation of Li3InCl6 ·2H2O hydrates, which can effectively reduce the migration energy barrier of Li ions and offer reversible hydration/dehydration pathway. Finally, an ASSLB, assembled with reheated‐Li2.8Zr0.2In0.8Cl6 after humidity exposure, single‐crystal LiNi0.8Mn0.1Co0.1O2 and Li‐In alloy, exhibits capacity retention of 71% after 500 cycles under 1 C at 25 °C. This novel high‐humidity‐tolerant chloride electrolyte is expected to greatly carry forward the ASSLBs industrialization. Herein, the humidity tolerance of halide solid‐state electrolytes using the soft acid element In‐doped Li2ZrCl6 is investigated and found that hc‐Li0.8Zr0.2In0.8Cl6 has high ionic conductivity, good thermal stability, and hygroscopic reversibility, which will greatly enhance the commercialization of all‐solid‐state lithium batteries.