Covalent Assembly of MoS2 Nanosheets with SnS Nanodots as Linkages for Lithium/Sodium‐Ion Batteries

Weak van der Waals interactions between interlayers of two-dimensional layered materials result in disabled across-interlayer electron transfer and poor layered structural stability, seriously deteriorating their performance in energy applications. Herein, we propose a novel covalent assembly strategy for MoS2 nanosheets to realize unique MoS2 /SnS hollow superassemblies (HSs) by using SnS nanodots as covalent linkages. The covalent assembly based on all-inorganic and carbon-free concept enables effective across-interlayer electron transfer, facilitated ion diffusion kinetics, and outstanding mechanical stability, which are evidenced by experimental characterization, DFT calculations, and mechanical simulations. Consequently, the MoS2 /SnS HSs exhibit superb rate performance and long cycling stability in lithium-ion batteries, representing the best comprehensive performance in carbon-free MoS2 -based anodes to date. Moreover, the MoS2 /SnS HSs also show excellent sodium storage performance in sodium-ion batteries.