Exploring the structure evolution of MoS₂ upon Li/Na/K ion insertion and the origin of the unusual stability in...

The recent revival of research on Na and K ion batteries has two benefits. It not only provides alternate energy storage technologies to Li ion batteries with potential cost advantages but also enhances our understanding of charge storage through systematic studies on alkali-metal ion batteries with increasing insertion ion sizes. Using MoS2 as a model material, the structure evolution upon the uptake of Li, Na, and K ions are compared through in situ TEM. Despite their larger size, insertion of K ions shows both the better electrochemical and structural stability. To understand this paradoxical and counter-intuitive phenomenon, in situ XRD is carried out to examine the phase transitions of MoS2 upon ion insertion, while ex situ TEM is further applied to closely examine the structures at the nanoscale. Complementary DFT calculations are performed to understand the kinetic/thermodynamic origins of the unusual stability. The result reveal that the less electrovalent K-S bond favors the intercalation process, resulting in preservation of the layered structure for stable cycling. This study provides a structural insight to design stable electrodes for the K-ion batteries.