Deciphering the role of Van der Waals heterostructures in enhancing layered perovskite anodes for high-performance lithium-ion batteries

Abstract

Organic-inorganic hybrid halide perovskites have recently gained significant attention due to their outstanding optoelectronic property. However, the application of halide perovskite for lithium-ion batteries (LIBs) is still in its infancy with inferior battery performance and blurry reaction mechanism. This study presents a layered perovskite Li2(C2H7NO3S)2CuCl4 (LTCC) and deciphers the role of Van der Waals heterostructures in high-performance anode material for LIBs. The LTCC anode can achieve a remarkable specific capacity of 861 mA h/g at 0.1 A/g after 100 cycles and maintains a high discharging capacity of 548 mA h/g over 550 cycles at 1.0 A/g, which currently exhibits outstanding cycling stability among perovskite-type anode materials for LIBs. Comprehensive characterizations illustrate the partially reversible conversion reaction of LTCC anode to form CuCl, LiCl, and Li taurine during the lithiation process. Furthermore, experimental and theoretical results reveal that the unique Van der Waals heterostructure of LTCC can enhance the structure stability and boost the Li-ion adsorption/transportation ability, thus accounting for the superior lithium storage performance. This study not only sheds light on the accurate electrochemical reaction mechanism of perovskite-type materials but also provides valuable insights for developing high-performance perovskite-based anodes in LIBs.