Electrical, Mechanical, and Capacity Percolation Leads to High-Performance MoS₂/Nanotube Composite Lithium Ion Battery Electrodes

Advances in lithium ion batteries would facilitate technological developments in areas from electrical vehicles to mobile communications. While two-dimensional systems like MoS₂ are promising electrode materials due to their potentially high capacity, their poor rate capability and low cycle stability are severe handicaps. Here, we study the electrical, mechanical, and lithium storage properties of solution-processed MoS₂/carbon nanotube anodes. Nanotube addition gives up to 10¹⁰-fold and 40-fold increases in electrical conductivity and mechanical toughness, respectively. The increased conductivity results in up to a 100× capacity enhancement to ∼1200 mAh/g (∼3000 mAh/cm³) at 0.1 A/g, while the improved toughness significantly boosts cycle stability. Composites with 20 wt % nanotubes combine high reversible capacity with excellent cycling stability (e.g., ∼950 mAh/g after 500 cycles at 2 A/g) and high rate capability (∼600 mAh/g at 20 A/g). The conductivity, toughness, and capacity scale with nanotube content according to percolation theory, while the stability increases sharply at the mechanical percolation threshold. We believe that the improvements in conductivity and toughness obtained after addition of nanotubes can be transferred to other electrode materials, such as silicon nanoparticles.