High-energy Batteries Research Articles

Design Strategies of Spinel Oxide Frameworks Enabling Reversible Mg-Ion Intercalation.

ConspectusReversible Mg2+ intercalation in metal oxide frameworks is a key enabler for an operational Mg-ion battery with high energy density needed for the next generation of energy storage technologies. While functional Mg-ion batteries have been achieved in structures with soft anions (e.g., S2- and Se2-), they do not meet energy density requirements to compete with the current rechargeable lithium-ion batteries due to their low insertion potentials. It emphasizes the necessity of finding an oxide-based cathode that operates at high potentials. A leading hypothesis to explain the limited availability of oxide Mg-ion cathodes is the belief that Mg2+ has sluggish diffusion kinetics in oxides due to strong electrostatic interactions between the Mg2+ ions and oxide anions in the lattice. From this assessment, it can be hypothesized that such rate limiting kinetic shortcomings can be mitigated by tailoring an oxide framework through creating less stable Mg2+-O2- coordination.Based on theoretical calculations and preliminary experimental data, oxide spinels have been identified as promising cathode candidates with storage capacity, insertion potential, and cation mobility that meet the requirements for a secondary Mg-ion battery. However, spinels with a single redox metal, such as MgCr2O4 or MgMn2O4, were not found to demonstrate sufficiently reversible Mg-ion intercalation at high redox potentials when coupled with nonaqueous Mg-electrolytes. Therefore, a materials development effort was initiated to design, synthesize, and evaluate a new class of solid-solution oxide spinels that can satisfy the required properties needed to create a sustainable Mg-ion cathode. These were designed by bringing together electrochemically active metals with stable redox potentials and charged states against the electrolyte, for instance, Mn3+, in combination with a structural stabilization component, typically Cr3+. Furthermore, common spinel structural defects that degrade performance, i.e., antisite inversion, were controlled to see correlation between structures and electrochemical overpotentials, thus controlling overall hysteresis. The designed materials were characterized by both short- and long-range structure in both ex situ and in situ modes to confirm the nature of solid-solution and to correlate structural changes and redox activity to electrochemical performance. Consistent and reproducible results were observed for facile bulk Mg2+-ion activity without phase transformations, leading to enhanced energy storage capability based on reversible intercalation of Mg2+, enabled by understanding the variables that control the electrochemical performance of the spinel oxide. Based on these observations, with proper materials design, it is possible to develop an oxide cathode material that has many of the desired properties of a Li-ion intercalation cathode, representing a significant mile marker in the quest for high energy density Mg-ion batteries.This Account describes strategies for the design and development of new spinel oxide intercalation materials for high-energy Mg-ion battery cathodes through a combination of theoretical and experimental approaches. We will review the key factors that govern the kinetics of Mg2+ diffusion in spinel oxides and illustrate how material complexity correlates with the electrochemical Mg2+ activity in oxides and is supported by secondary characterization. The understanding gained from the fundamental studies of cation diffusion in oxide cathodes will be beneficial for chemists and materials scientists who are developing rechargeable batteries.

An inorganic-rich but LiF-free interphase for fast charging and long cycle life lithium metal batteries

Li metal batteries using Li metal as negative electrode and LiNi1-x-yMnxCoyO2 as positive electrode represent the next generation high-energy batteries. A major challenge facing these batteries is finding electrolytes capable of forming good interphases. Conventionally, electrolyte is fluorinated to generate anion-derived LiF-rich interphases. However, their low ionic conductivities forbid fast-charging. Here, we use CsNO3 as a dual-functional additive to form stable interphases on both electrodes. Such strategy allows the use of 1,2-dimethoxyethane as the single solvent, promising superior ion transport and fast charging. LiNi1-x-yMnxCoyO2 is protected by the nitrate-derived species. On the Li metal side, large Cs+ has weak interactions with the solvent, leading to presence of anions in the solvation sheath and an anion-derived interphase. The interphase is surprisingly dominated by cesium bis(fluorosulfonyl)imide, a component not reported before. Its presence suggests that Cs+ is doing more than just electrostatic shielding as commonly believed. The interphase is free of LiF but still promises high performance as cells with high LiNi0.8Mn0.1Co0.1O2 loading (21 mg/cm2) and low N/P ratio (~2) can be cycled at 2C (~8 mA/cm2) with above 80% capacity retention after 200 cycles. These results suggest the role of LiF and Cs-containing additives need to be revisited.

Enhanced lithiophilicity via bismuth-infused framework for advanced lithium metal batteries

Utilizing carbon materials as 3D lithium (Li) hosts hold a significant interest in constructing high-energy batteries. However, there are ongoing challenges associated with these frameworks owing to their poor Li affinity. Recent advancements, including alloying reactions with precious metals like silver (Ag) and gold (Au), have emerged as a promising technique to enhance the electrochemical performance of these host materials. Nevertheless, the search for cost-effective alternatives remains a pressing demand. Herein, this work employed galvanic displacement (GD) to integrate bismuth into disordered porous carbon (Bi-DPC) and optimized across different concentrations (0.01, 0.05, 0.1 M). As a result, the Li deposition onto the Bi-DPC surface exhibited dendrite-free planar morphologies, revealing an outstanding electrochemical performance, including a high CE of around 100 % over more than 100 cycles. These findings underscore the potential of Bi-infused porous carbon as a promising alternative for enhancing Li deposition processes.

Designing electrolytesand interphases for high-energy lithium batteries.

High-energy and stable lithium-ion batteries are desired for next-generation electric devices and vehicles. To achieve their development, the formation of stable interfaces on high-capacity anodes and high-voltage cathodes is crucial. However, such interphases in certain commercialized Li-ion batteries are not stable. Due to internal stresses during operation, cracks are formed in the interphase and electrodes; the presence of such cracks allows for the formation of Li dendrites and new interphases, resulting in a decay of the energy capacity. In this Review, we highlight electrolyte design strategies to form LiF-rich interphases in different battery systems. In aqueous electrolytes, the hydrophobic LiF can extend the electrochemical stability window of aqueous electrolytes. In organic liquid electrolytes, the highly lithiophobic LiF can suppress Li dendrite formation and growth. Electrolyte design aimed at forming LiF-rich interphases has substantially advanced high-energy aqueous and non-aqueous Li-ion batteries. The electrolyte and interphase design principles discussed here are also applicable to solid-state batteries, as a strategy to achieve long cycle life under low stack pressure, as well as to construct other metal batteries.

Superionic Conductor Enabled Composite Lithium with High Ionic Conductivity and Interfacial Wettability for Solid‐State Lithium Batteries

AbstractThe urgent demand for high energy and safety batteries has generated the rapid development of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) type solid‐state lithium metal batteries. However, severe dendritic lithium growth, which is caused by poor interfacial contact of the Li/LLZTO interface and loss of electrical contact during cycles due to low intrinsic Li+ diffusion coefficient of lithium, greatly hampers its practical application. Here, from the point of view of reducing surface tension and improving ion diffusion of lithium, a composite lithium anode (CLA) with high wettability and ion diffusion coefficient is prepared by adding GaP into molten lithium, thus strengthening the CLA/LLZTO interface even in cycling. As envisioned, compared to pure lithium, CLA presents lower surface tension, larger adhesion work, and higher ion diffusion coefficient, ensuring close contact of the CLA/LLZTO interface. Therefore, the assembled symmetric cells exhibit a low area specific resistance of 4.5 Ω cm2, a large critical current density of 2.5 mA cm−2, and ultra‐long lifespan of 5700 h at 0.3 mA cm−2 at 25 °C. Meanwhile, full cells coupled with LiFePO4 cathode show a high‐capacity retention of 97.32% after 490 cycles at 1C. This work provides a new solution to the interfacial challenges of solid‐state lithium‐metal batteries.

Lithium Bis(fluorosulfonyl)imide for Stabilized Interphases on Conjugated Dicarboxylate Electrode.

Carbonyl-based negative electrodes have received considerable interest in the domain of rechargeable lithium batteries, owing to their superior feasibility in structural design, enhanced energy density, and good environmental sustainability. Among which, lithium terephthalate (LiTPA) has been intensively investigated as a negative electrode material in the past years, in light of its relatively stable discharge plateau at low potentials (ca. 1.0 V vs Li/Li+) and high specific capacity (ca. 290 mAh g-1). However, its cell performances are severely limited owing to the poor quality of the solid-electrolyte-interphase (SEI) layer generated therein. Here, we report the utilization of lithium bis(fluorosulfonyl)imide (LiFSI) as an electrolyte salt for forming a Li-ion permeable SEI layer on the LiTPA electrode and subsequently improving the cyclability and rate performance of the LiTPA-based cells. Our results show that, differing from the reference electrolyte containing the lithium hexafluorophosphate (LiPF6) salt, the electrochemical reductions of the FSI- anions occur prior to the lithiation processes of LiTPA electrode, which is capable of building an inorganic-rich SEI layer containing lithium fluoride (LiF) and lithium sulfate (Li2SO4). Consequently, the lithium metal (Li°)||LiTPA cell shows significantly improved cycling performance than the LiPF6-based reference cell. This work provides useful insight into the reductive processes of the FSI- anions on negative electrodes, which could spur the deployment of highly sustainable and high-energy rechargeable lithium batteries.

Structural and surface engineering promotes Zn-ion energy storage capability of commercial carbon cloth

Aqueous Zn-ion hybrid supercapacitors (AZHSCs) combining the advantages of high-energy batteries and high-power supercapacitors see a bright future, but they still suffer from the poor capacity of carbonic cathodes. Herein, a functionalized porous carbon cloth (denoted as FPCC) electrode is demonstrated based on commercial carbon cloth (denoted as CC) tuning by structural and surface engineering. The constructed exfoliated porous carbon layer and the negatively charged functionalized interface not only increase the electrical double layer capacitance but also favor the chemical adsorption of Zn2+ to obtain additional pseudocapacitance. Consequently, the FPCC electrode delivers a high capacity of 0.16 mAh cm−2 at 4 mA cm−2, which is 923.8 times higher than CC, and a long cycle life (85.0% capacity retention after 30 000 cycles). More importantly, the Zn//FPCC AZHSC possesses an impressive energy density (3.3 mWh cm−3) and power density (240 mW cm−3), superior to many advanced batteries and supercapacitors. The quasi-solid-state device is also assembled as a demo. This modification strategy may provide new opportunities for high-performance AZHSCs.

Dynamically Evolving Multifunctional Protective Layer for Highly Stable Potassium Metal Anodes.

The construction of an artificial protective layer is an effective method to solve the issues, such as uncontrolled dendrite growth and an unstable solid electrolyte interphase, at the K metal anode. This study proposes a new dynamic evolution strategy that integrates the advantages of previous in situ and ex situ fabrication processes. A multifunctional protective layer enriched with K-Ge alloy is prepared on the K metal electrode by simple surface modification and in situ reduction via an electrochemical process. The protective layer has good potassiophilicity, mechanical flexibility, and high ionic conductivity, which can inhibit dendrite growth and reduce side reactions. The protected K electrode with a protective layer exhibits dendrite-free K plating/striping behavior, and the symmetric cell can run stably for over 1000 h at 1 mA cm-2 and 1 mAh cm-2. Notably, full cells based on this electrode also present excellent rate and cycling performance compared to those of the bare K electrode. This peculiar strategy will open a new avenue for metal anode protection and can be extended to other high-energy battery systems.

Monothetic and conductive network and mechanical stress releasing layer on micron-silicon anode enabling high-energy solid-state battery

Monothetic and conductive network and mechanical stress releasing layer on micron-silicon anode enabling high-energy solid-state battery

Inorganic Polysulfide Chemistries for Better Energy Storage Systems.

ConspectusSulfur-based cathode materials have become a research hot spot as one of the most promising candidates for next-generation, high-energy lithium batteries. However, the insulating nature of elemental sulfur or organosulfides has become the biggest challenge that leads to dramatic degradation and hinders their practical application. The disadvantage is more obvious for all-solid-state battery systems, which require both high electronic and ionic migration at the same sites to realize a complete electrochemical reaction. In addition to adding conductive components into the cathode composites, another effective way to realize high-reversibility sulfur-based cathodes is by optimizing the inherent nature of sulfur-based materials to make them "conductive". Inorganic polysulfide materials including polysulfide molecules, selenium-sulfur solid solutions, and (lithium) metal polysulfides are promising, as they have different structures that can make them intrinsically conductive or becoming conductive during lithiation. They all contain at least one -S-S- bridged bond, which is the intrinsic structural characteristic and the source of the chemical properties of these polysulfide compounds. For example, by balancing the conductivity and reversible capacity, researchers in the US National Aeronautics and Space Administration (NASA) have shown that 500 Wh/kg solid-state Li-Se/S batteries can power cars and even electric aircraft.We have long been focusing on the inorganic polysulfide component, reported the selenium-sulfur solid solutions, the first sulfur-rich phosphorus polysulfide molecules, and followed the research of metal polysulfide components. The proposed Account summarizes our current knowledge of the fundamental aspects of inorganic polysulfides in energy storage systems based on state-of-the-art publications on this topic. Both fast electron and ion migrations within the electrode materials are vital to achieving high-energy batteries. We begin by illustrating effective approaches to enhance the electronic/ionic conductivity of sulfur-based electrode materials. We then present some basic observations and properties (especially the intrinsic high conductivities) of the inorganic polysulfide electrode materials. The key chemical and structural factors dictating their conductive and electrochemical behaviors will be discussed. Finally, we show the advantages and broad applications of inorganic polysulfides in energy storage areas. The proposed Account will provide an insightful perspective on the current knowledge of inorganic polysulfide materials, as well as their future research directions and development potential, serving as a keynote reference for researchers in the field of energy storage.

Cationic Defect-Modulated Li-Ion Migration in High-Voltage Li-Metal Batteries.

Li metal exhibits high potential as an anode material for next-generation high-energy density batteries. However, the nonuniform transport of Li+ ions causes Li-dendrite growth at the metal electrode, leading to severe capacity decay and a short cycling life. In this study, negatively charged lithiophilic sites (such as cationic metal vacancies) were used as hosts to regulate the atomic-scale Li+-ion deposition in Li-metal batteries (LMBs). As a proof of concept, three-dimensional (3D) carbon nanofibers (CNFs) decorated with negatively charged TiNbO4 grains (labeled CNF/nc-TNO) were confirmed to be promising Li hosts. Cationic vacancies caused by the carbothermal reduction of Nb5+ and Ti4+ ions generated a negatively charged fiber surface and strong electrostatic interactions that guided the Li+-ion flux to the shadowed areas underneath the fiber and throughout the fibrous mat. Consequently, circumferential Li-metal plating was observed in the CNF/nc-TNO host, even at a high current density of 10 mA cm-2. Moreover, CNF/nc-TNO asymmetric cells delivered a significantly more robust and stable Coulombic efficiency (CE) (99.2% over 380 cycles) than cells comprising electrically neutral CNFs without cationic defects (which exhibits rapid failure after 20 cycles) or Cu foil (which exhibits rapid CE decay, with a CE of 87.1% after 100 cycles). Additionally, CNF/nc-TNO exhibited high stability and low-voltage hysteresis during repeated Li plating/stripping (for over 4000 h at 2 mA cm-2) with an areal capacity of 2 mAh cm-2. It was further paired with high-voltage LiNi0.8Co0.1Mn0.1 (NCM811) cathodes, and the full cells showed long-term cycling (220 cycles) with a CE of 99.2% and a steady rate capability.

Applications, prospects and challenges of metal borides in lithium sulfur batteries

Although the lithium-sulfur (Li-S) battery has a theoretical capacity of up to 1675 mA h g−1, its practical application is limited owing to some problems, such as the shuttle effect of soluble lithium polysulfides (LiPSs) and the growth of Li dendrites. It has been verified that some transition metal compounds exhibit strong polarity, good chemical adsorption and high electrocatalytic activities, which are beneficial for the rapid conversion of intermediate product in order to effectively inhibit the “shuttle effect”. Remarkably, being different from other metal compounds, it is a significant characteristic that both metal and boron atoms of transition metal borides (TMBs) can bind to LiPSs, which have shown great potential in recent years. Here, for the first time, almost all existing studies on TMBs employed in Li-S cells are comprehensively summarized. We firstly clarify special structures and electronic features of metal borides to show their great potential, and then existing strategies to improve the electrochemical properties of TMBs are summarized and discussed in the focus sections, such as carbon-matrix construction, morphology control, heteroatomic doping, heterostructure formation, phase engineering, preparation techniques. Finally, the remaining challenges and perspectives are proposed to point out a direction for realizing high-energy and long-life Li-S batteries.

External Pressure Affecting Dendrite Growth and Dissolution in Lithium Metal Batteries During Cycles.

Lithium (Li) metal has garnered significant attention as the preferred anode for high-energy lithium metal batteries. However, safety concerns arising from the growth of Li dendrites have hindered the advancement of Li metal batteries. In this study, we first elucidate the impact of external pressure and internal stress on dendrite growth and dissolution behavior of Li metal batteries during continuous charging-discharging cycles, employing a developed electrochemomechanical phase-field model. A typical parameter is defined to calculate the amount of dead Li that affects the electrochemical performance of Li metal batteries during multiple cycles. The underlying mechanisms of dendrites observed from in situ experiments are explained through the developed phase-field model. After charging/discharging, dendrites with a treelike structure yield a greater amount of dead Li compared to those with a needlelike configuration. Increasing the pressure appropriately can effectively reduce the growth points of dendrites and suppress the Li dendrite growth. Excessive pressure not only induces dendritic fractures that lead to the formation of dead Li but also undermines the battery performance. The accumulated internal stress might threaten the structural stability of the Li metal, thereby influencing the evolution of the Li dendrite morphology. A reasonable strategy is proposed to strike a balance between external pressure and the growth and dissolution of Li dendrites. These findings offer valuable insights into the judicious application of pressure to mitigate the advancement of electroplating reactions.

Bismuth and Chlorine Dual-Doped Perovskite Chloride as a Phase-Structure-Stable and Moisture-Resistant Solid Electrolyte for Chloride Ion Batteries.

Perovskite chloride, an anion conductor, is a promising candidate to be a solid electrolyte for high-energy and sustainable chloride ion batteries (CIB). However, it suffers from poor structural stability at low temperature and in ambient conditions, which leads to its transformation from an ionic conductor to an insulator. Herein, a bismuth and chlorine dual doping strategy is developed to stabilize the cubic structure of CsSnCl3 in harsh environments. The as-prepared dual-doped CsSn0.9 Bi0.1 Cl3.1 material with an optimized composition maintains its cubic structure at the extremely low temperature of 213K for 10 days and at 40% relative humidity for 50 days, while the undoped cubic material deteriorates and transforms to a monoclinic phase under these conditions in less than 1 day. Consequently, the dual doping achieves efficient chloride ion conduction that is superior to single bismuth doping due to the introduction of interstitial chlorine facilitating chloride ion transport. Importantly, the practicality of the as-prepared solid electrolyte is demonstrated in different symmetric solid cells and by various CIBs using the organic electrode couple, a multivalent metal chloride cathode, or a new high-voltage metal oxychloride cathode.

La-Al Intermetallic Alloy Anode for Realizing High-Energy Fluoride-Ion Battery

An all-solid-state fluoride-ion battery is one of the promising candidates for the next-generation high-energy batteries owing to the high theoretical energy density. However, the practical capacities of anodes are significantly low compared with cathodes, and therefore it is an urgent task to develop new anode materials for fluoride-ion batteries. Here, we show that the LaAl3 alloy anode delivers a reversible high capacity of 298 mAh g−1 with only 0.66% capacity fading per cycle. By using atomic-resolution scanning transmission electron microscopy combined with electron energy-loss spectroscopy, we investigate the structural and chemical evolution of LaAl3. We find that LaAl3 is firstly decomposed into LaF3 and AlF3 nanocrystals, forming the nanoscale network of the F– ion conduction path owing to the high ionic conductivity of LaF3. In the subsequent cycles, the redox reaction of Al/AlF3 nanocrystals solely proceeds, contributing to the reversible high capacity. Our findings should open new avenues for realizing high-energy fluoride-ion batteries.

Two-Step Redox Reactions of Iodine Molecules in Single-Walled Carbon Nanotubes for High Capacity and High Energy Batteries

Two-Step Redox Reactions of Iodine Molecules in Single-Walled Carbon Nanotubes for High Capacity and High Energy Batteries

Asymmetric Electrode Design for High-Area Capacity and High-Energy Efficiency Hybrid Zn Batteries.

Compared to Zn-air batteries, by integrating Zn-transition metal compound reactions and oxygen redox reactions at the cell level, hybrid Zn batteries are proposed to achieve higher energy density and energy efficiency. However, attaining relatively higher energy efficiency relies on controlling the discharge capacity. At high area capacities, the proportion of the high voltage section can be neglected, resulting in a lower energy efficiency similar to that of Zn-air batteries. Here, a high-loading integrated electrode with an asymmetric structure and asymmetric wettability is fabricated, which consists of a thick nickel hydroxide (Ni(OH)2) electrode layer with vertical array channels achieving high capacity and high utilization, and a thin NiCo2O4 nanopartical-decorated N-doped graphene nanosheets (NiCo2O4/N-G)catalyst layer with superior oxygen catalytic activity. The asymmetric wettability satisfies the wettability requirements for both Zn-Ni and Zn-air reactions. The hybrid Zn battery with the integrated electrode exhibits a remarkable peak power density of 141.9mWcm-2, superior rate performance with an energy efficiency of 71.4% even at 20mAcm-2, and exceptional cycling stability maintaining a stable energy efficiency of ≈84% at 2mAcm-2 over 100 cycles (400 h).

Improve the compatibility of sulfolane-graphite with the synergetic additives

The high voltage stability (> 5.5 V) makes sulfolane (SL) an excellent electrolyte solvent candidate for high specific energy lithium-ion batteries. However, the stable solid electrolyte interphase (SEI) cannot be generated on the surface of graphite particles with SL, limiting its application. To solve the interface incompatibility, we introduce fluoroethylene carbonate (FEC) and lithium nitrate (LiNO3) in SL-based electrolyte for constructing an inorganic-rich SEI on graphite. The comprehensive characterizations and simulations demonstrate that combined effect of additives facilitates the formation of additive-derived LiF-Li3N enhanced inorganic-rich SEI. The proposed electrolyte shows stable cycling performances with 324.89 mAh/g and 97.93 % after 50 cycles in Li/graphite half-cells, compared with the capacity of 24.54 mAh/g and the capacity retention of 19.4 % in SL-without additives. Importantly, the electrolyte system obtains a capacity retention of 71 % and the capacity of (127.93 mAh/g) is higher than that without additives (110.21 mAh/g) at 4.4 V after 200 cycles. This work solves the incompatibility of SL-graphite with low-cost additives, and is beneficial to realize the commercial application of sulfolane in high specific energy batteries.

Synergetic Sn Incorporation-Zn Substitution in Copper-Based Sulfides Enabling Superior Na-Ion Storage.

Transition-metal sulfides have been regarded as perspective anode candidates for high-energy Na-ion batteries. Their application, however, is precluded severely by either low charge storage or huge volumetric change along with sluggish reaction kinetics. Herein, an effective synergetic Sn incorporation-Zn substitution strategy is proposed based on copper-based sulfides. First, Na-ion storage capability of copper sulfide is significantly improved via incorporating an alloy-based Sn element. However, this process is accompanied by sacrifice of structural stability due to the high Na-ion uptake. Subsequently, to maintain the high Na-ion storage capacity, and concurrently improve cycling and rate capabilities, a Zn substitution strategy (taking partial Sn sites) is carried out, which could significantly promote Na-ion diffusion/reaction kinetics and relieve mechanical strain-stress within the crystal framework. The synergetic Sn incorporation and Zn substitution endow copper-based sulfides with high specific capacity (≈560 mAh g-1 at 0.5 A g-1 ), ultrastable cyclability (80 k cycles with ≈100% capacity retention), superior rate capability up to 200 A g-1 , and ultrafast charging feature (≈4 s per charging with ≈190 mAh g-1 input). This work provides in-depth insights for developing superior anode materials via synergetic multi-cation incorporation/substitution, aiming at solving their intrinsic issues of either low specific capacity or poor cyclability.

Rational Design of High-Loading Electrodes with Superior Performances Toward Practical Application for Energy Storage Devices.

High-loading electrodes play a crucial role in designing practical high-energy batteries as they reduce the proportion of non-active materials, such as current separators, collectors, and battery packaging components. This design approach not only enhances battery performance but also facilitates faster processing and assembly, ultimately leading to reduced production costs. Despite the existing strategies to improve rechargeable battery performance, which mainly focus on novel electrode materials and high-performance electrolyte, most reported high electrochemical performances are achieved with low loading of active materials (<2mgcm-2). Such low loading, however, fails to meet application requirements. Moreover, when attempting to scale up the loading of active materials, significant challenges are identified, including sluggish ion diffusion and electron conduction kinetics, volume expansion, high reaction barriers, and limitations associated with conventional electrode preparation processes. Unfortunately, these issues are often overlooked. In this review, the mechanisms responsible for the decay in the electrochemical performance of high-loading electrodes are thoroughly discussed. Additionally, efficient solutions, such as doping and structural design, are summarized to address these challenges. Drawing from the current achievements, this review proposes future directions for development and identifies technological challenges that must be tackled to facilitate the commercialization of high-energy-density rechargeable batteries.