Temperature-Dependent Vapor Infiltration of Sulfur into Highly Porous Hierarchical Three-Dimensional Conductive Carbon Networks for Lithium Ion Battery Applications

[Image: see text] Hierarchical, conductive, porous, three-dimensional (3D) carbon networks based on carbon nanotubes are used as a scaffold material for the incorporation of sulfur in the vapor phase to produce carbon nanotube tube/sulfur (CNTT/S) composites for application in lithium ion batteries (LIBs) as a cathode material. The high conductivity of the carbon nanotube-based scaffold material, in combination with vapor infiltration of sulfur, allows for improved utilization of insulating sulfur as the active material in the cathode. When sulfur is evenly distributed throughout the network via vapor infiltration, the carbon scaffold material confines the sulfur, allowing the sulfur to become electrochemically active in the context of an LIB. The electrochemical performance of the sulfur cathode was further investigated as a function of the temperature used for the vapor infiltration of sulfur into the carbon scaffolds (155, 175, and 200 °C) in order to determine the ideal infiltration temperature to maximize sulfur loading and minimize the polysulfide shuttle effect. In addition, the nature of the incorporation of sulfur at the interfaces within the 3D carbon network at the different vapor infiltration temperatures will be investigated via Raman, scanning electron microscopy/energy dispersive X-ray, and X-ray photoelectron spectroscopy. The resulting CNTT/S composites, infiltrated at each temperature, were incorporated into a half-cell using Li metal as a counter electrode and a 0.7 M LiTFSI electrolyte in ether solvents and characterized electrochemically using cyclic voltammetry measurements. The results indicate that the CNTT matrix infiltrated with sulfur at the highest temperature (200 °C) had improved incorporation of sulfur into the carbon network, the best electrochemical performance, and the highest sulfur loading, 8.4 mg/cm(2), compared to the CNTT matrices infiltrated at 155 and 175 °C, with sulfur loadings of 4.8 and 6.3 mg/cm(2), respectively.