Enhanced Li‐Ion‐Storage Performance of MoS 2 through Multistage Structural Design

Abstract Inspired by a folded protein, multistage structural MoS 2 is designed as an advanced anode material for lithium‐ion batteries (LIBs). Density functional theory (DFT) calculations are initially performed, demonstrating that the ideal primary structure (P−MoS 2 ) has saw‐tooth‐like edges terminated by Mo atoms and the desired secondary structure (C−MoS 2 ) may form via crumpling. For the latter, more exposed (002) planes exist within the wrinkled parts, creating more active sites and promoting isotropic Li + insertion. Importantly, the rate capability and capacity of a MoS 2 anode are enhanced after such a P−MoS 2 to C−MoS 2 transition: a superb specific capacity of 1490 mAh/g for C−MoS 2 at 0.1 A/g (vs. 1083 mAh/g for P−MoS 2 ), an excellent cycling stability (858 mAh/g after 450 cycles at 0.5 A/g), and an improved rate capability of 591 mAh/g at 1 A/g (vs. 465 mAh/g) are documented. The curving effects and mechanical properties of a single C−MoS 2 particle are further visualized by in situ TEM. Drastically enlarged spacing changes upon Li‐insertion and high elasticity are confirmed, which lead to enhanced LIB performances and the excellent mechanical strength of C−MoS 2 . The present multistage design of a MoS 2 structure should pave the way toward high‐energy MoS 2 anode materials for future LIBs.