Cation Defect-Engineered Boost Fast Kinetics of Two-Dimensional Topological Bi 2 Se 3 Cathode for High-Performance Aqueous Zn-Ion Batteries.

The challenge with aqueous zinc-ion batteries (ZIBs) lies in finding suitable cathode materials that can provide high capacity and fast kinetics. Herein, two-dimensional topological Bi 2 Se 3 with acceptable Bi-vacancies for ZIBs cathode (Cu-Bi 2-x Se 3 ) is constructed through one-step hydrothermal process accompanied by Cu heteroatom introduction. The cation-deficient Cu-Bi 2-x Se 3 nanosheets (∼ 4 nm) bring improved conductivity from large surface topological metal states contribution and enhanced bulk conductivity. Besides, the increased adsorption energy and reduced Zn 2+ migration barrier demonstrated by density-functional theory (DFT) calculations illustrate the decreased Coulombic ion-lattice repulsion of Cu-Bi 2-x Se 3 . Therefore, Cu-Bi 2-x Se 3 exhibits both enhanced ion and electron transport capability, leading to more carrier reversible insertion proved by in-situ synchrotron X-ray diffraction (SXRD). These features endow Cu-Bi 2-x Se 3 with sufficient specific capacity (320 mA h g -1 at 0.1 A g -1 ), high-rate performance (97 mA h g -1 at 10 A g -1 ), and reliable cycling stability (70 mA h g -1 at 10 A g -1 after 4000 cycles). Furthermore, quasi-solid-state fiber-shaped ZIBs employing the Cu-Bi 2-x Se 3 cathode demonstrate respectable performance and superior flexibility even under high mass loading. This work implements a conceptually innovative strategy represented by cation defect design in topological insulator cathode for achieving high-performance battery electrochemistry. This article is protected by copyright. All rights reserved.