Aluminum-ion batteries (AIBs) are regarded as promising candidates for post-lithium-ion batteries due to their lack of flammability and electrochemical performance comparable to other metal-ion batteries. The lack of suitable cathode materials, however, has hindered the development of high-performing AIBs. Sulfur is a cost-efficient material, having distinguished electrochemical properties, and is considered an attractive cathode material for AIBs. Several pioneering reports have shown that aluminum-sulfur batteries (ASBs) exhibit superior electrochemical capacity over other cathode materials for AIBs. However, a rapid decay in the capacity is a huge barrier for their practical applications. Here, we have demonstrated systematically for the first time that the two-dimensional layered materials (e.g. MoS2, WS2, and BN) can serve as fixers of S and sulfide compounds during repeated charge/discharge processes; BN/S/C displays the highest capacity of 532 mAh g-1 (at a current density of 100 mA g-1) compared with the current state-of-the-art cathode material for AIBs. Further, we could improve the life-span of ASBs to an unprecedented 300 cycles with a high Coulombic efficiency of 94.3%; discharge plateaus at ~1.15 V vs. AlCl4-/Al was clearly observed during repeated charge/discharge cycling. We believe that this work opens up a new method for achieving high-performing ASBs.

Department of Materials Science and Engineering Research Institute of Advanced Materials Seoul National University Seoul 08826 Republic of Korea

Electronic Materials Center Korea Institute of Science and Technology Seoul 136 791 Republic of Korea

Regional Centre of Advanced Technologies and Materials Faculty of Science Palacky University in Olomouc Šlechtitelů 27 783 71 Olomouc Czech Republic

Small and Medium Enterprises Support Center Korea Institute of Science and Technology Seoul Republic of Korea

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