may offer noteworthy cost saving and safety improvement compared to its counterparts. Additionally, aluminum has a very negative redox potential (≈1.676 V vs standard hydrogen electrode (SHE)) and a small electrochemical equivalent (0.336 g Ah −1 ), which make it one of the ideal elements for rechargeable batteries. However, the previous efforts have encountered numerous issues over the past few years, such as the cathode material disintegration, [12,14] low discharge voltage, [8] capacitive behavior without discharge voltage plateaus. [15,16] There is no doubt that some of recent works have explored a series of new electrode materials, such as V 2 O 5 , [8] TiO 2 , [9] fluorinated natural graphite, [15] polymers, [16] and Prussian blue analogues (PBAs). [12] The previous work has revealed that Al ions can insert into TiO 2 nanotube arrays and PBAs in aqueous solution. But the discharge capacity of these materials is too low. Very recently, the works from our group at University of Science and Technology Beijing (USTB) and Dai and co-workers at Stanford University found that rechargeable aluminum-ion batteries using graphite materials cathode had a very high charge/discharge voltage plateau around 2.0 V versus Al 3+ /Al. [12,17] The charge/discharge reaction happens through the intercalation and deintercalation of AlCl 4 − into interlayer space of graphite materials.Herein, we report for the first time, the design of Ni 3 S 2 / graphene microflakes composite as a novel cathode material for rechargeable aluminum-ion batteries. The battery runs through the electrochemical deposition and dissolution of aluminum at the anode, and the intercalation and deintercalation of Al 3+ cations in the cathode. The unique advantage of Ni 3 S 2 /graphene microflakes composite lies in the low charge-transfer impedance, which represents a high rate of intercalation and deintercalation of ions. Additionally, we find that there is a dissociation process of Al 2 Cl 7 − during charge process, and the active material transforms from monocrystal to polycrystal at the same time. The battery exhibits a high discharge voltage plateau (≈1.0 V vs Al/AlCl 4 − ), a discharge capacity of over 60 mA h g −1 , a high coulombic efficiency of about 99% , and a high rate capability, suggesting that it is a favorable cathode material for high-performance aluminumion batteries.

Due to their small footprint and flexible siting, rechargeable batteries are attractive for energy storage systems. A super-valent battery based on aluminium ion intercalation and deintercalation is proposed in this work with VO2 as cathode and high-purity Al foil as anode. First-principles calculations are also employed to theoretically investigate the crystal structure change and the insertion-extraction mechanism of Al ions in the super-valent battery. Long cycle life, low cost and good capacity are achieved in this battery system. At the current density of 50 mAg−1, the discharge capacity remains 116 mAhg−1 after 100 cycles. Comparing to monovalent Li-ion battery, the super-valent battery has the potential to deliver more charges and gain higher specific capacity.

Rechargeable aluminum-ion batteries (AIBs) are regarded as promising candidates for post-lithium energy storage systems (ESSs). For addressing the critical issues in the current liquid AIB systems, here a flexible solid-state AIB is established using a gel-polymer electrolyte for achieving robust electrodeelectrolyte interfaces. Different from utilization of solid-state systems for alleviating the safety issues and enhancing energy density in lithium-ion batteries, employment of polymeric electrolytes mainly focuses on addressing the essential problems in the liquid AIBs, including unstable internal interfaces induced by mechanical deformation and production of gases as well as unfavorable separators. Particularly, such gel electrolyte enables the solid-state AIBs to present an ultra-fast charge capability within 10 s at current density of 600 mA g −1 . Meanwhile, an impressive specific capacity ≈120 mA h g −1 is obtained at current density of 60 mA g −1 , approaching the theoretical limit of graphite-based AIBs. In addition to the well-retained electrochemical performance below the ice point, the solid-state AIBs also hold great stability and safety under various critical conditions. The results suggest that such new prototype of solid-state AIBs with robust electrode-electrolyte interfaces promises a novel strategy for fabricating stable and safe flexible ESSs.

For significantly increasing the energy densities to satisfy the growing demands, new battery materials and electrochemical chemistry beyond conventional rocking-chair based Li-ion batteries should be developed urgently. Rechargeable aluminum batteries (RABs) with the features of low cost, high safety, easy fabrication, environmental friendliness, and long cycling life have gained increasing attention. Although there are pronounced advantages of utilizing earth-abundant Al metals as negative electrodes for high energy density, such RAB technologies are still in the preliminary stage and considerable efforts will be made to further promote the fundamental and practical issues. For providing a full scope in this review, we summarize the development history of Al batteries and analyze the thermodynamics and electrode kinetics of nonaqueous RABs. The progresses on the cutting-edge of the nonaqueous RABs as well as the advanced characterizations and simulation technologies for understanding the mechanism are discussed. Furthermore, major challenges of the critical battery components and the corresponding feasible strategies toward addressing these issues are proposed, aiming to guide for promoting electrochemical performance (high voltage, high capacity, large rate capability, and long cycling life) and safety of RABs. Finally, the perspectives for the possible future efforts in this field are analyzed to thrust the progresses of the state-of-the-art RABs, with expectation of bridging the gap between laboratory exploration and practical applications.

A new Al-ion battery based on an affordable and nontoxic liquid electrolyte made from molten AlCl/urea was assembled. As the cathode material, natural graphite shows two well-defined discharge voltage plateaus at about 1.9 and 1.5 V with a high specific capacity of 93 mA h g and excellent coulombic efficiency (>99%). The attractive capacity (about 78 mA h g) is retained even at a high current density of 1000 mA g. Moreover, no faster fading in capacity is observed after 500 cycles. This electrolyte could provide a new system for Al ion batteries, which can be used for large scale energy storage, owing to its cost advantages, high-rate capability and durability.