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Benefiting from high volumetric capacity, environmental friendliness, and high safety, aluminum-ion batteries (AIBs) are considered to be promising battery system among emerging electrochemical energy storage technologies. As an important component of AIBs, the cathode material is crucial to decide the energy density and cycle life of AIBs. However, single-component cathode materials are unable to achieve a balance between cycling stability and rate performance. In recent years, research on heterostructure cathode materials has gained significant attention in AIBs. By harnessing the synergistic effects of heterostructure, the shortcomings of individual materials can be overcome, contributing to improved conductivity and structural stability. This review offers a detailed insight into the Al-storage mechanism of heterostructure cathodes, and provides an overview of the current research progresses on heterostructure cathode materials for AIBs. Starting from the relationship between the microstructure and electrochemical performance of heterostructure materials, the different structure design strategies are elaborated. Besides, the challenges faced by heterostructure are summarized, and their potential impact on the future of the energy storage industry is anticipated. This review provides the guidelines for the future research of heterostructure as cathode materials for AIBs.
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Nonaqueous aluminum-ion batteries (AIBs) provide advantages, such as high energy density, enhanced safety, and reduced corrosion, making them ideal for advanced energy storage solutions. A key challenge faced by AIBs is the lack of suitable cathode materials for rapid Al-ion insertion /extraction. Herein, K2Mn[Fe(CN)6] 2H2O (KMHCF) is innovatively chosen as a model to investigate the aluminum storage performance of Prussian blue analogues in nonaqueous AIBs. As anticipated, the KMHCF allows for reversible aluminum storage and exhibits characteristic charge/discharge plateaus. Furthermore, carbon combined highly crystalline KMHCF (HC-KMHCF@C) is synthesized through a chelator-assisted preparation method in combination with an in situ carbon compositing technique. With reduced [Fe(CN)6]4⻠defects, lower interstitial water content, and enhanced conductivity, HC-KMHCF@C exhibits a high aluminum storage capacity (146.2 mAh g⻹ at 0.5 A g⻹) and satisfactory cycling performance (maintaining 86.4 mAh g⻹ after 800 cycles). The electrochemical reaction mechanism of HC-KMHCF@C is investigated in detail. During the initial charge, K⺠ions are extracted, shifting the structure from monoclinic to cubic. In subsequent cycles, reversible Al3+ insertion and extraction cause the structure to alternate between monoclinic and cubic phases.
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Aluminum-ion batteries (AIBs), as electrochemical energy storage technologies, are advantageous because of their high theoretical specific capacity, lightweightness, zero pollution, safety, inexpensiveness, and abundant resources, which make them recent research hot spots. However, their electrolyte issues significantly limit their commercialization. The electrolyte choices for AIBs are significantly limited, and most of the available choices do not facilitate the three-electron-transfer reaction of Al3+/Al. Thus, this review presents an overview of recent advances in electrolytes, as well as modification strategies for AIBs, to clarify the limitations of existing AIB electrolytes and offer guidance for improving their performances. Furthermore, the advantages as well as limitations and possible solutions for each electrolyte are discussed, after which the future of AIB electrolytes is envisioned.
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Aqueous aluminum-ion batteries have many advantages such as their safety, environmental friendliness, low cost, high reserves and the high theoretical specific capacity of aluminum. So aqueous aluminum-ion batteries are potential substitute for lithium-ion batteries. In this paper, the current research status and development trends of cathode and anode materials and electrolytes for aqueous aluminum-ion batteries are described. Aiming at the problem of passivation, corrosion and hydrogen evolution reaction of aluminum anode and dissolution and irreversible change of cathode after cycling in aqueous aluminum-ion batteries. Solutions of different research routes such as ASEI (artificial solid electrolyte interphase), alloying, amorphization, elemental doping, electrolyte regulation, etc and different transformation mechanisms of anode and cathode materials during cycling have been summarized. Moreover, it looks forward to the possible research directions of aqueous aluminum-ion batteries in the future. We hope that this review can provide some insights and support for the design of more suitable electrode materials and electrolytes for aqueous aluminum-ion batteries.
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In aqueous aluminum-ion batteries (AAIBs), the insertion/extraction chemistry of Al3+ often leads to poor kinetics, whereas the rapid diffusion kinetics of hydronium ions (H3O+) may offer the solution. However, the presence of considerable Al3+ in the electrolyte hinders the insertion reaction of H3O+. Herein, we report how oxygen-deficient α-MoO3 nanosheets unlock selective H3O+ insertion in a mild aluminum-ion electrolyte. The abundant oxygen defects impede the insertion of Al3+ due to excessively strong adsorption, while allowing H3O+ to be inserted/diffused through the Grotthuss proton conduction mechanism. This research advances our understanding of the mechanism behind selective H3O+ insertion in mild electrolytes.
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In pursuit of high-performance aluminum-ion batteries, the selection of a suitable positive electrode material assumes paramount importance, and fluorinated graphene (FG) nanostructures have emerged as an exceptional candidate. In the scope of this study, a flexible tantalum foil is coated with FG to serve as the positive electrode for aluminum-ion batteries. FG positive electrode demonstrates a remarkable discharge capacity of 109â mA h g-1 at a current density of 200â mA g-1, underscoring its tremendous potential for energy storage applications. Concurrently, the FG positive electrode exhibits a discharge capacity of 101â mA h g-1 while maintaining an impressive coulombic efficiency of 95 % over 300â cycles at a current density of 200â mA g-1, which benefiting from the significant structure of FG. The results of the in-situ Raman spectroscopy signified the presence of intercalation/de-intercalation processes of AlCl4 - behavior within the FG layers.
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Aluminum-ion batteries (AIBs) have become a research hotspot in the field of energy storage due to their high energy density, safety, environmental friendliness, and low cost. However, the actual capacity of AIBs is much lower than the theoretical specific capacity, and their cycling stability is poor. The exploration of energy storage mechanisms may help in the design of stable electrode materials, thereby contributing to improving performance. In this work, molybdenum disulfide (MoS2) was selected as the host material for AIBs, and carbon nanofibers (CNFs) were used as the substrate to prepare a molybdenum disulfide/carbon nanofibers (MoS2/CNFs) electrode, exhibiting a residual reversible capacity of 53 mAh g-1 at 100 mA g-1 after 260 cycles. The energy storage mechanism was understood through a combination of electrochemical characterization and first-principles calculations. The purpose of this study is to investigate the diffusion behavior of ions in different channels in the host material and its potential energy storage mechanism. The computational analysis and experimental results indicate that the electrochemical behavior of the battery is determined by the ion transport mechanism between MoS2 layers. The insertion of ions leads to lattice distortion in the host material, significantly impacting its initial stability. CNFs, serving as a support material, not only reduce the agglomeration of MoS2 grown on its surface, but also effectively alleviate the volume expansion caused by the host material during charging and discharging cycles.
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Aqueous aluminum-ion batteries (AIBs) have great potential as devices for future large-scale energy storage systems due to the cost efficiency, environmentally friendly nature, and impressive theoretical energy density of Al. However, currently, available materials used as anodes for aqueous AIBs are scarce. In this study, a novel sol-gel method was used to synthesize nitrogen-doped titanium dioxide (N-TiO2) as a potential anode material for AIBs in water. The annealed N-TiO2 showed a high discharge capacity of 43.2 mAh g-1 at a current density of 3 A g-1. Analysis of the electrode kinetics revealed that the N-TiO2 anodes exhibited rapid diffusion of aluminum ions, low resistance to charge transfer, and high electronic conductivity, enabling good rate performance. The successful implementation of a nitrogen-doping strategy provides a promising approach to enhance the electrochemical characteristics of electrode materials for aqueous AIBs.
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The two-dimensional (2D) MXenes with sufficient interlayer spacing are promising cathode materials for aluminum-ion batteries (AIBs), yet the electrostatic repulsion effect between the surface negative charges and the active anions (AlCl4 - ) hinders the intercalation of AlCl4 - and is usually ignored. Here, we propose a charge regulation strategy for MXene cathodes to overcome this challenge. By doping N and Co, the zeta potential is gradually transformed from negative (Ti3 C2 Tx ) to near-neutral (Ti3 CNTx ), and finally positive (Ti3 CNTx @Co). Therefore, the electrostatic repulsion force can be greatly weakened between Ti3 CNTx and AlCl4 - , or even formed a strong electrostatic attraction between Ti3 CNTx @Co and AlCl4 - , which can not only accommodate more AlCl4 - ions in the Ti3 CNTx @Co interlayers to increase the capacity, but also solve the stacking and expansion problems. As a result, the optimized Al-MXene battery exhibits an ultrahigh capacity of up to 240â mAh g-1 (2-4â times the capacity of graphite cathode, 60-120â mAh g-1 ) and a potential ultrahigh energy density (432â Wh kg-1 , 2-4â times the value of graphite, 110-220â Wh kg-1 ) based on the mass of cathode materials, comparable to LiFePO4 -based lithium-ion batteries (350-450â Wh kg-1 , based on the mass of LiFePO4 ).
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Rechargeable aluminum-ion batteries (AIBs) have emerged as a promising candidate for energy storage applications and have been extensively investigated over the past few years. Due to their high theoretical capacity, nature of abundance, and high safety, AIBs can be considered an alternative to lithium-ion batteries. However, the electrochemical performance of AIBs for large-scale applications is still limited due to the poor selection of cathode materials. Transition metal dichalcogenides (TMDs) have been regarded as appropriate cathode materials for AIBs due to their wide layer spacing, large surface area, and distinct physiochemical characteristics. This mini-review provides a succinct summary of recent research progress on TMD-based cathode materials in non-aqueous AIBs. The latest developments in the benefits of utilizing 3D-printed electrodes for AIBs are also explored.
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The battery performance declines significantly in severely cold areas, especially discharge capacity and cycle life, which is the most significant pain point for new energy consumers. To address this issue and improve the low-temperature characteristic of aluminum-ion batteries, in this work, polydopamine-derived N-doped carbon nanospheres are utilized to modify the most promising graphite material. More active sites are introduced into graphite, more ion transport channels are provided, and improved ionic conductivity is achieved in a low-temperature environment. Due to the synergistic effect of the three factors, the ion diffusion resistance is significantly reduced and the diffusion coefficient of aluminum complex ions in the active material become larger at low temperatures. Therefore, the battery delivers an improved capacity retention rate from 23% to 60% at -20 °C and excellent ultra-long cycling stability over 5500 cycles at -10 °C. This provides a novel strategy for constructing low-temperature aluminum-ion batteries with high energy density, which is conducive to promoting the practicality of aluminum-ion batteries.
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Restricted by the available energy storage modes, currently rechargeable aluminum-ion batteries (RABs) can only provide a very limited experimental capacity, regardless of the very high gravimetric capacity of Al (2980 mAh g-1 ). Here, a novel complexation mechanism is reported for energy storage in RABs by utilizing 0D fullerene C70 as the cathode. This mechanism enables remarkable discharge voltage (≈1.65 V) and especially a record-high reversible specific capacity (750 mAh g-1 at 200 mA g-1 ) of RABs. By means of in situ Raman monitoring, mass spectrometry, and density functional theory (DFT) calculations, it is found that this elevated capacity is attributed to the direct complexation of one C70 molecule with 23.5 (super)halogen moieties (superhalogen AlCl4 and/or halogen Cl) in average, forming (super)halogenated C70 ·(AlCl4 )m Cln-m complexes. Upon discharging, decomplexation of C70 ·(AlCl4 )m Cln-m releases AlCl4 - /Cl- ions while preserving the intact fullerene cage. This work provides a new route to realize high-capacity and long-life batteries following the complexation mechanism.
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Aluminum-ion batteries have garnered an extensive amount of attention due to their superior electrochemical performance, low cost, and high safety. To address the limitation of battery performance, exploring new cathode materials and understanding the reaction mechanism for these batteries are of great significance. Among numerous candidates, multiple structures and valence states make manganese-based oxides the best choice for aqueous aluminum-ion batteries (AAIBs). In this work, a new cathode consists of γ-MnO2 with abundant oxygen vacancies. As a result, the electrode shows a high discharge capacity of 481.9 mAh g-1 at 0.2 A g-1 and a sustained reversible capacity of 128.6 mAh g-1 after 200 cycles at 0.4 A g-1. In particular, through density functional theory calculation and experimental comparison, the role of oxygen vacancies in accelerating the reaction kinetics of H+ has been verified. This study provides insights into the application of manganese dioxide materials in aqueous AAIBs.
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Constructing robust anode with strong aluminophilicity and rapid desolvation kinetics is essential for achieving high utilization, long-term durability, and superior rate performance in Al metal-based energy storage, yet remains largely unexplored. Herein, molybdenum nanoparticles embedded onto nitrogen-doped graphene (Mo@NG) are designed and prepared as Al host to regulate the deposition behavior and achieve homogeneous Al plating/stripping. The monodispersed Mo nanoparticles reduce the desolvation energy barrier and promote the deposition kinetics of Al. Additionally, Mo nanoparticles act as aluminophilic nucleation sites to minimize the Al nucleation overpotential, further guiding uniform and dense Al deposition. As a result, the dual-functional Mo@NG endows Al anodes with low voltage hysteresis, reversible Al plating/stripping with high coulombic efficiency, and excellent high-rate capability under 5 mA cm-2 . Moreover, the as-designed Al metal full batteries deliver a high capacity retention of 92.8% after 3000 cycles at 1 A g-1 . This work provides an effective solution to optimize the electrochemical properties of Al metal anode from the perspective of desolvation and deposition reactions, towards the development of high-safety and long-cycling aluminum-ion batteries.
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Developing cathode materials with high specific capability and excellent electrochemical performance is crucial for the advancement of aluminum-ion batteries, which leverage the high theoretical energy density of aluminum metal anodes. In this paper, we investigated the interaction ofAlCl4cluster and Al atom with AlN (-100) and (001) monolayer using density functional theory to assess the applicability of AlN as cathode material for aluminum-ion batteries. The results show that the AlN (001) monolayer is the most effective for adsorbing and accommodatingAlCl4clusters. Moreover, the AlN (001) monolayer maintains metallic behavior at different concentrations of theAlCl4cluster, laying the foundation for its battery application. The theoretical storage capacity of theAlCl4cluster is 105.93mAhg-1,which exceeds that of the Al/graphite battery. The formation energy ofAlCl4-intercalated AlN compounds is -2.74 eV, and the intercalant gallery height is moderate. Furthermore, the diffusion barrier of 0.19 eV forAlCl4cluster between the AlN (001) monolayer provides high rate capability. The results indicate that AlN monolayer may be a potential cathode material for aluminum-ion batteries.
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Solid-state zinc ion batteries (ZIBs) and aluminum-ion batteries (AIBs) are deemed as promising candidates for supplying power in wearable devices due to merits of low cost, high safety, and tunable flexibility. However, their wide-scale practical application is limited by various challenges, down to the material level. This Review begins with elaboration of the root causes and their detrimental effect for four main limitations: electrode-electrolyte interface contact, electrolyte ionic conductivity, mechanical strength, and electrochemical stability window of the electrolyte. Thereafter, various strategies to mitigate each of the described limitation are discussed along with future research direction perspectives. Finally, to estimate the viability of these technologies for wearable applications, economic-performance metrics are compared against Li-ion batteries.
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Liquid electrolyte systems of aluminum-ion batteries (AIBs) have restrictive issues, such as high moisture sensitivity, strong corrosiveness, and battery leakage, so researchers have turned their attention to developing high safety, leak-free polymer electrolytes. However, the stability of the active factor of AIB systems is difficult to maintain with most of polymeric frameworks due to the special Al complex ion balance in chloroaluminate salts. Based on this, this work clarified the feasibility and specific mechanism of using polymers containing functional groups with lone pair electrons as frameworks of solid-state electrolytes for AIBs. As for the polymers reacting unfavorably with AlCl3, they cannot be used as the frameworks directly due to the decrease or even disappearance of chloroaluminate complex ions. In contrast, a class of polymers represented by polyacrylamide (PAM) can interact with AlCl3 and provide ligands, which not only have no effect on the activity of Al species but also provide chloroaluminate complex ions through complexation reactions. According to DFT calculations, amide groups tend to coordinates with AlCl2 + via O atoms to form [AlCl2(AM)2]+ cations, while disassociating chloroaluminate anions. Furthermore, the PAM-based solid-state and quasi-solid-state gel polymer electrolytes were also prepared to investigate their electrochemical properties. This work is expected to provide new theoretical and practical directions for the further development of polymer electrolytes for AIBs.
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Organic electrode materials (OEMs) have shown enormous potential in ion batteries because of their varied structural components and adaptable construction. As a brand-new energy-storage device, rechargeable aluminum-ion batteries (RAIBs) have also received a lot of attention due to their high safety and low cost. OEMs are expected to stand out among many traditional RAIB cathode materials. However, how to improve the electrochemical performance of OEMs in RAIBs on a laboratory scale is still challenging. This work reviews and discusses the uses of conductive polymers, carbonyl compounds, imine polymers, polycyclic aromatic hydrocarbons, organic frameworks, and other organic materials as the cathodes of RAIBs, as well as energy-storage mechanisms and research progress. It is hoped that this Review can provide the design guidelines for organic cathode materials with high capacity and great stability used in aluminum-organic batteries and develop more efficient organic energy storage cathodes.
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Rechargeable aluminum-ion batteries (RAIBs) have emerged as a promising battery storage technology owing to their cost-effectiveness, operational safety, and high energy density. However, their actual capacity is substantially lower than their true capacity and their cycling stability is poor. Therefore, understanding the energy-storage mechanism may contribute to the successful design of a stable electrode material, on which the performance can be optimized. The aim of this study is to investigate AlCl4 - ions in transition metal cathode materials and mechanisms that enable for their high-energy-storage potential and low Coulombic efficiency. Results of theoretical analysis and experimental verification show that a multi-ion transport mechanism is responsible for the electrochemical behavior of the battery. The lattice distortion of CoSe2 caused by AlCl4 - ion intercalation, has a considerable effect on the initial stability of the battery. MXene as a support material reduces the size of CoSe2 growing on its surface, effectively inhibiting the lattice distortion caused by the interaction with the aluminum-anion complex, thus addressing the issues of poor reversibility, cycle instability, and low Coulombic efficiency of the battery. Hence, understanding the impact of MXene on the battery may aid in further improving the design of electrode materials.
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Al ion batteries (AIBs) are attracting considerable attention owing to high volumetric capacity, low cost, and high safety. However, the strong electrostatic interaction between Al3+ and host lattice leads to discontented cycling life and inferior rate capability. Herein, a new strategy of employing water molecules contained VOPO4 ·H2 O to boost Al3+ migration via the charge shielding effect of water is reported. It is revealed that VOPO4 ·H2 O with water lubrication effect and smaller steric hindrance owns high capacity and fast Al3+ diffusion, while the loss of unstable water upon cycling leads to a rapid performance degradation. To address this problem, ultrathin VOPO4 ·H2 O@MXene nanosheets are fabricated via the formed TiOV bond between VOPO4 ·H2 O and MXene. The MXene aided exfoliation results in enhanced VOwater bond strength between H2 O and VOPO4 that endows the obtained composite with strong water holding ability, contributing to the extraordinary cycling stability. Consequently, the VOPO4 ·H2 O@MXene delivers a high discharge potential of 1.8 V and maintains discharge capacities of 410 and 374.8 mAh g-1 after 420 and 2000 cycles at the current densities of 0.5 and 1.0 A g-1 , respectively. This work provides a new understanding of water-contained AIBs cathodes and vital guidance for developing high-performance AIBs.