Unusual Hybrid Magnesium Storage Mechanism in a New Type of Bi₂O₂CO₃ Anode.

Abstract

Bismuth and bismuth-based compounds have been extensively studied as anodes as prospective candidates for rechargeable magnesium batteries (rMBs). However, the unsatisfactory magnesium-storage capability caused by the typical alloying reaction mechanism severely restricts the practical option for anodes in rMBs. Herein, polyaniline intercalated Bi₂O₂CO₃ nanosheets are prepared by an effective interlayer engineering strategy to fine-tune the layer structure of Bi₂O₂CO₃, achieving enhanced magnesium-storage capacity, rate performance, as well as long cycle life. Excitedly, a stepwise insertion-conversion-alloying reaction is aroused to stabilize the performance, which is elucidated by <i>in</i>/<i>ex situ</i> investigations. Moreover, first-principles calculations confirm that the coupling of Bi₂O₂CO₃ and polyaniline not only increases the conductivity induced by the strong density of states and the interior self-built-in electric field but also significantly reduces the energy barrier of Mg shuttles. Our findings shed light on exploring new electrode materials with an appropriate working mechanism toward high-performance rechargeable batteries.