Tremella-like Vanadium Tetrasulfide as a High-Performance Cathode Material for Rechargeable Aluminum Batteries

Abstract

Rechargeable aluminum batteries (RABs) are gaining widespread attention for large-scale energy storage applications as a result of their high energy densities, high security, and abundance. The key to sustain the progress of RABs lies in the quest for the proper cathode materials with prominent capacity and reversible cycle life. Herein, we propose a tremella-like VS 4 as a cathode material aiming to tackle this problem. Obtained from a morphology modification process, VS 4 with a unique nanosheet structure provides sufficient active sites for intercalation and conversion reactions, shortens the transport paths for charge carrier ions, and facilitates the infiltration process for electrolyte. The RAB with the VS 4 cathode exhibits excellent electrochemical performance, including outstanding specific capacity (407.9 mAh g −1 ) and stable cycling performance (∼300 cycles at a high current density). The energy storage mechanism has been comprehensively investigated and is confirmed to be a combination of the intercalation/ deintercalation of Al 3+ and AlCl 4 − ions and conversion reaction by various techniques and DFT calculation. Our study not only provides a peculiar and simple strategy for the rational design of metal sulfide cathode materials with high capacity and long-term stability but also proposes a specific energy storage mechanism that guides the development of cathode materials of RABs in the future.

Strategy for enhancement of magnesium ion diffusion in a vanadium tetra sulfide-layered structure for rechargeable magnesium batteries

“…These results confirm and align with the trend of other reported chalcogenide materials that cathodes of VS 4 can uphold better cycling stability at a higher current density, which is further enhanced after Ni substitution. 39 Fig. 6h 5%Ni–VS 4 showed a much longer cycling life of up to 1500 cycles at a current density of 500 mA g −1 within the potential window of 0–2.1 V and retained a capacitance of around 45 mA h g −1 .…”

Advanced V-based materials for multivalent-ion storage applications

“…Transition metal sulfides, e.g., VS 4 in nanowires or auricular shapes, were also reported to deliver good Al-storage performance. A channel-rich VS 4 nanowire achieved 252.5 mAh g -1 at 100 mA g -1 after five activation cycles and held 138.9 mAh g -1 after 100 cycles at 0.4 A g -1 [97] . An auricular VS 4 retained 322.2 mAh g -1 at 200 mA g -1 after 120 cycles [98] .…”

Configurational Entropy Strategy Enhanced Structure Stability Achieves Robust Cathode for Aluminum Batteries

“…[ 1 ] In theory, the Al anode can deliver a superior volumetric capacity (≈8046 mAh cm −3 ) and high gravimetric capacity (≈2980 mAh g −1 ). [ 2 ] In previous works, various cathode materials, such as carbon materials, [ 3 ] metal oxides, [ 4 ] sulfides, [ 5 ] selenides, [ 6 ] and tellurides, [ 7 ] have been widely exploited in RABs. Despite this, the development of cathode materials with high reversible capacity and long service life is still limited to match the Al anode because of the strong interaction between the large‐size Al‐complex ions and the host.…”