Enhanced Li‐ion storage of MoS2 through multistage structural design

Inspired by a folded protein, the multistage structural MoS2 are designed as the advanced anode materials for lithium‐ion batteries (LIBs). The density functional theory (DFT) calculations are initially performed, demonstrating that an ideal primary structure (P‐MoS2) has the saw‐tooth‐like edges terminated by Mo atoms and the desired secondary structure (C‐MoS2) 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 MoS2 anode are enhanced after such P‐MoS2 to C‐MoS2 transition: superb specific capacity of 1490 mAh/g for C‐MoS2 at 0.1 A/g (vs. 1083 mAh/g for P‐MoS2), 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‐MoS2 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‐MoS2. The present multistage design of a MoS2 structure should pave the way toward high‐energy MoS2 anode materials for future LIBs.