Cation Defect‐Engineered Boost Fast Kinetics of Two‐Dimensional Topological Bi2Se3 Cathode for High‐Performance Aqueous Zn‐Ion Batteries

• Published in: Advanced materials (Weinheim) 2023-12, Vol.35 (51), p.n/a
• Main Authors: Zong, Yu, Chen, Haichao, Wang, Jinsong, Wu, Menghua, Chen, Yu, Wang, Liyu, Huang, Xinliang, He, Hongwei, Ning, Xin, Bai, Zhongchao, Wen, Wen, Zhu, Daming, Ren, Xiaochuan, Wang, Nana, Dou, Shixue
• Format: Article
• Language: English
• Subjects: Cathodes; cation defect; Cations; Copper; Density functional theory; Design defects; Electrochemistry; Electrode materials; Electron transport; in situ synchrotron X‐ray diffraction; Kinetics; Materials science; Synchrotrons; Topological insulators; two‐dimensional bismuth selenide; zinc ion batteries
• ISSN: 0935-9648; 1521-4095
• DOI: 10.1002/adma.202306269

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 Bi2Se3 with acceptable Bi‐vacancies for ZIBs cathode (Cu‐Bi2−xSe3) is constructed through one‐step hydrothermal process accompanied by Cu heteroatom introduction. The cation‐deficient Cu‐Bi2−xSe3 nanosheets (≈4 nm) bring improved conductivity from large surface topological metal states contribution and enhanced bulk conductivity. Besides, the increased adsorption energy and reduced Zn2+ migration barrier demonstrated by density‐functional theory (DFT) calculations illustrate the decreased Coulombic ion‐lattice repulsion of Cu‐Bi2−xSe3. Therefore, Cu‐Bi2−xSe3 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‐Bi2−xSe3 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‐Bi2−xSe3 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. The challenge with aqueous zinc‐ion batteries (ZIBs) lies in the design of suitable cathode materials. Herein, two‐dimensional topological Bi2Se3 with acceptable cation vacancies for ZIBs cathode is constructed through one‐step hydrothermal process, which exhibits both enhanced ion and electron transport capability. The remarkable reversible charge storage capacity points to its promising strategy for achieving high performance aqueous zinc‐ion batteries.