Atomic-scale tandem regulation of anionic and cationic migration for long-life alkali metal batteries
Abstract Atomic-scale regulation of both cationic and anionic transport is of great significance in membrane-based separation technologies. Ionic transport regulation techniques could also play a crucial role in developing high-performance alkali metal batteries such as alkali metal-sulfur and alkali metal-selenium batteries, which suffer from the non-uniform transport of alkali metal ions and detrimental shuttling of polysulfide/polyselenide (PS) anions. These obstacles can cause severe growth of alkali metal dendrites and the irreversible consumption of active cathodes, leading to capacity decay and short cycling life. Herein, we report long-life alkali metal batteries enabled by atomic-scale tandem regulation of the migration of both alkali metal cations (Li+/Na+) and PS anions using negatively charged Ti0.87O2 nanosheets with Ti atomic vacancies. The shuttling of PS anions has been effectively eliminated via a robust electrostatic repulsion between the negatively charged nanosheets and PS anions. The negatively charged nanosheets can also regulate the migration of Li+/Na+ ions to ensure a homogeneous ion flux through efficient but light adhesion of Li+/Na+ ions within the nanosheets. The atomic Ti vacancies act as sub-nanometre pores to provide fast diffusion channels for Li+/Na+ ions. Therefore, eradication of PS shuttling and stable Li/Na-ion diffusion without compromising the fast transport of Li+/Na+ ions has been achieved for long-life alkali metal-sulfur and alkali metal-selenium batteries. This work provides a facile and effective strategy to regulate the transport of both cations and anions for developing advanced rechargeable batteries by using two-dimensional vacancy-enhanced materials.