Customizable Crystalline-Amorphous Rectifying Heterostructure Cathodes for Durable and Super-Fast Zinc Storage

Abstract

The development of high-capacity, quick-charging, long-lasting cathodes are crucial for the advancement of aqueous zinc ion battery (AZIBs). However, it is still challenging for most developed electrodes to simultaneously satisfy these interconnected requirements. Starting from the customized high-crystalline material by physical vapor transport method, this report unlocks the design of unique VSSe-V2O5 core-shell composite with the crystalline-amorphous characteristic, which was enabled by electrochemical scanning of VSSe to form the amorphous heterogeneous surface. In detail, the superior conductivity of metallic VSSe core directly facilitate rapid electron transfer. Meanwhile, the amorphous V2O5 shell presents prominent hydrophilic and zincophilic traits that bolster spontaneous adsorption of zinc ion. When at the heterogeneous interface, the interaction between VSSe and V2O5 generates a unique built-in electric field, enhancing rectification behavior from the core outward. Benefited from such crystalline-amorphous core-shell heterogeneous structure, this electrode displays superior rate performance with a discharge capacity of 162 mAh g-1 at ultrahigh current density of 50 A g-1. Beyond that, it enables delivering a specific capacity of 176 mAh g-1 at 30 A g-1 with a remarkable 17000-cycle lifespan and a capacity retention of 93%. In addition, such customized paradigm can be extended to other VS0.5Se1.5, VS1.5Se0.5, and MnS0.5Se0.5 materials. This work underscores the impressive storage performance of the crystalline-amorphous rectifying heterogeneous cathode, and highlighting the surface amorphous heterogenization of customized material as a promising direction for developing robust cathodes and advanced aqueous zinc-ion batteries.