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Over the past several decades, the number of electric vehicles (EVs) has continued to increase. Projections estimate that worldwide, more than 125 million EVs will be on the road by 2030. At the heart of these advanced vehicles is the lithium-ion (Li-ion) battery which provides the required energy storage. This paper presents and compares key components of Li-ion batteries and describes associated battery management systems, as well as approaches to improve the overall battery efficiency, capacity, and lifespan. Material and thermal characteristics are identified as critical to battery performance. The positive and negative electrode materials, electrolytes and the physical implementation of Li-ion batteries are discussed. In addition, current research on novel high energy density batteries is presented, as well as opportunities to repurpose and recycle the batteries.

AbstractMetal–organic frameworks (MOFs) and covalent organic frameworks (COFs) as two burgeoning families of crystalline porous materials (CPMs) have been extensively investigated and applied in various fields on account of their enticing features as large surface area, controllable crystalline structure and highly ordered pores/channels. However, the greatest stumbling block to their widespread application in electrochemical energy storage systems is the inferior electrical conductivity. Therefore, numerous efforts have been exerted on exploiting the advantages and remedying the disadvantages. In this review, we mainly focus on pristine MOFs and COFs, emphasize the recent progress and highlight the milestones of their applications in the fields of lithium-ion batteries, lithium–sulfur batteries, lithium–air batteries and supercapacitors. We hope to provide a constructive view of the structure–activity relationship between CPMs and energy storage systems and promote their future development.Graphic Abstract

Lithium‐sulfur (Li‐S) batteries are considered as one of the most promising energy storage systems for next‐generation electric vehicles because of their high‐energy density. However, the poor cyclic stability, especially at a high sulfur loading, is the major obstacles retarding their practical use. Inspired by the nacre structure of an abalone, a similar configuration consisting of layered carbon nanotube (CNT) matrix and compactly embedded sulfur is designed as the cathode for Li‐S batteries, which are realized by a well‐designed unidirectional freeze‐drying approach. The compact and lamellar configuration with closely contacted neighboring CNT layers and the strong interaction between the highly conductive network and polysulfides have realized a high sulfur loading with significantly restrained polysulfide shuttling, resulting in a superior cyclic stability and an excellent rate performance for the produced Li‐S batteries. Typically, with a sulfur loading of 5 mg cm−2, the assembled batteries demonstrate discharge capacities of 1236 mAh g−1 at 0.1 C, 498 mAh g−1 at 2 C and moreover, when the sulfur loading is further increased to 10 mg cm−2 coupling with a carbon‐coated separator, a superhigh areal capacity of 11.0 mAh cm−2 is achieved. Lithium–sulfur batteries are one of the most promising energy storage systems for the next‐generation electric vehicles from the high theoretical energy density. From the unidirectional freeze‐drying approach, a nacre‐like carbon nanotube sheet is prepared and used as the cathode matrix. Such a structure with compact carbon nanotube matrix–sulfur configuration enables a considerably high performance at a high areal sulfur loading.

This book offers a comprehensive examination of Li-S batteries from the viewpoint of the materials used in their construction, the underlying electrochemical mechanisms and how this translates into the characteristics of Li-S batteries. The authors - noted experts in the field - outline the approaches and techniques required to model Li-S batteries. This book reviews the application of Li-S batteries for commercial use and explores many broader issues including the development of battery management systems to control the unique characteristics of Li-S batteries. The authors include information on sulfur cathodes, electrolytes and other components used in making Li-S batteries and examine the role of lithium sulfide, the shuttle mechanism and its effects, and degradation mechanisms.

Polyolefin separators comprising polyethylene and polypropylene have long been used in commercial Li‐ion batteries because of their electrochemical stability, robust mechanical properties, uniform pore structure, and cost‐effectiveness. However, conventional separators have limitations in withstanding harsh environmental conditions, such as elevated temperatures, owing to their poor mechanical durability. Moreover, with the development of advanced Li rechargeable batteries, these separators are required to overcome new challenges such as preventing the migration of polysulfide intermediates in Li–S batteries and inhibiting the formation of Li dendrites in Li metal batteries. Natural clay minerals have emerged as a viable solution to these issues owing to their porous structure, high mechanical strength, and abundant polysulfide‐capturing Lewis acid sites. However, the manner in which the structural characteristics of minerals influence the separator performance has not been extensively assessed, thereby impeding the development of separators for future high‐performance Li batteries. This review comprehensively outlines various clay minerals and their effects on the parameters and performance metrics of battery separators. Based on this review, a design guide is proposed for mineral‐based separators that could potentially be integrated into next‐generation Li batteries with high energy density and long‐term stability. This review examines how coating Li‐ion battery separators with 1D, 2D, and 3D structured natural clay minerals influences their electrochemical and mechanical performance. It classifies 15 types of clay minerals and highlights structure–property correlations to offer practical design strategies for high‐performance separators in next‐generation energy storage systems.

Sulfide solid electrolyte (SSE)‐based all‐solid‐state Li batteries (ASSLBs) can overcome the problems of low energy density and safety concern of current Li‐ion batteries. However, the practical application of SSE‐based ASSLBs is suffered from several problems, especially interfacial issues between Li metal anode (LMA) and SSEs. Therefore, in this study, the problems of the LMA–SSE interface and their corresponding solutions are reviewed. First, the interfacial problems are summarized, namely the side reactions of SSEs, the Li dendrite growth, and poor contact between the electrode and electrolyte. Second, the available strategies to improve the robustness of the interface are discussed, including the protection of the LMA, substitution of the LMA, and modification of SSEs. Third, the characterization methods used to analyze the morphological and compositional evolution of the interface during cycling are introduced. Finally, the limitations and future research directions are proposed. The interface between Li metal anode and sulfide solid electrolyte in all‐solid‐state Li batteries is suffered from side reactions, Li dendrites, and poor contact, which can be solved by the protection of Li metal anode, subsitution of Li metal anode, and modification of sulfide solid electrolytes.

Lithium–air batteries (LABs) possess the highest energy density among all energy storage systems, and have drawn widespread interest in academia and industry. However, many arduous challenges are still to be conquered, one of them is Li2CO3, which is a ubiquitous product in LABs. It is inevitably produced but difficult to decompose; therefore, Li2CO3 is perceived as the “Achilles’ heel of LABs”. Among various approaches to addressing the Li2CO3 issue, developing Li2CO3-decomposing redox mediators (RMs) is one of the most convenient and versatile, because they can be electrochemically oxidized at the gas cathode surface, then they diffuse to the solid-state products and chemically oxidize them, recovering the RMs to a pristine state and avoiding solid-state catalysts’ contact instability with Li2CO3. Furthermore, because of their function mechanism, they can double as catalysts for Li2O2/LiOH decomposition, which are needed in LABs/LOBs anyway regardless of Li2CO3 incorporation due to the sluggish kinetics of oxygen reduction/evolution reactions. This review summarizes the progress in Li2CO3-decomposing RMs, including halides, metal–chelate complexes, and metal-free organic compounds. The insights into and discrepancies in the mechanisms of Li2CO3 decomposition and corresponding catalysis processes are also discussed.

The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing operando high-resolution optical microscopy combined with non-equilibrium thermodynamics implemented in a multi-dimensional (1D+1D to 3D) phase-field modeling framework to reveal the rate-dependent spatial dynamics of phase separation and plating in graphite electrodes. Here we visualize and provide mechanistic understanding of the multistage phase separation, plating, inter/intra-particle lithium exchange and plated lithium back-intercalation phenomena. A strong dependence of intra-particle lithiation heterogeneity on the particle size, shape, orientation, surface condition and C-rate at the particle level is observed, which leads to early onset of plating spatially resolved by a 3D image-based phase-field model. Moreover, we highlight the distinct relaxation processes at different state-of-charges (SOCs), wherein thermodynamically unstable graphite particles undergo a drastic intra-particle lithium redistribution and inter-particle lithium exchange at intermediate SOCs, whereas the electrode equilibrates much slower at low and high SOCs. These physics-based insights into the distinct SOC-dependent relaxation efficiency provide new perspective towards developing advanced fast charge protocols to suppress plating and shorten the constant voltage regime. Improved understanding of the spatial dynamics in graphite electrodes is needed to improve fast-charging protocols for Li-ion batteries. Here, authors highlight that lithiation heterogeneity leads to early lithium plating onset and find distinct relaxation behaviors at various states of charge.

HighlightsThe electrochemical principles/mechanism of Li–S batteries and origin of the shuttle effect have been discussed.The efficient strategies have been summarized to inhibit the shuttle effect.The recent advances of inhibition of shuttle effect in Li–S batteries for all components from anode to cathode.Lithium–sulfur (Li–S) batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost. Nevertheless, the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value. Many methods were proposed for inhibiting the shuttle effect of polysulfide, improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries. Here, we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries. First, the electrochemical principles/mechanism and origin of the shuttle effect are described in detail. Moreover, the efficient strategies, including boosting the sulfur conversion rate of sulfur, confining sulfur or lithium polysulfides (LPS) within cathode host, confining LPS in the shield layer, and preventing LPS from contacting the anode, will be discussed to suppress the shuttle effect. Then, recent advances in inhibition of shuttle effect in cathode, electrolyte, separator, and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries. Finally, we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.

Development in high-rate electrode materials capable of storing vast amounts of charge in a short duration to decrease charging time and increase power in lithium-ion batteries is an important challenge to address. Here, we introduce a synthesis strategy with a series of composition-controlled NMC cathodes, including LiNi0.2Mn0.6Co0.2O2(NMC262), LiNi0.3Mn0.5Co0.2O2(NMC352), and LiNi0.4Mn0.4Co0.2O2(NMC442). A very high-rate performance was achieved for Mn-rich LiNi0.2Mn0.6Co0.2O2 (NMC262). It has a very high initial discharge capacity of 285 mAh g−1 when charged to 4.7 V at a current of 20 mA g−1 and retains the capacity of 201 mAh g−1 after 100 cycles. It also exhibits an excellent rate capability of 138, and 114 mAh g−1 even at rates of 10 and 15 C (1 C = 240 mA g−1). The high discharge capacities and excellent rate capabilities of Mn-rich LiNi0.2Mn0.6Co0.2O2 cathodes could be ascribed to their structural stability, controlled particle size, high surface area, and suppressed phase transformation from layered to spinel phases, due to low cation mixing and the higher oxidation state of manganese. The cathodic and anodic diffusion coefficient of the NMC262 electrode was determined to be around 4.76 × 10−10 cm2 s−1 and 2.1 × 10−10 cm2 s−1, respectively.