Manipulating the Conversion Kinetics of Polysulfides by Engineering Oxygen p‐Band of Halloysite for Improved Li‐S Batteries

Polar oxides are widely used as the cathodes to impede the shuttle effect in lithium-sulfur batteries, but suffer from the sluggish desorption and conversion of polysulfides due to too strong affinity of polysulfides on oxygen sites. Herein, employing halloysite as a model, an approach to overcome these shortcomings is proposed via engineering oxygen p-band center by loading titanium dioxide nanoparticles onto Si-O surface of halloysite. Using density functional theory calculations, it is predicted that electron transfer from titanium dioxide nanoparticles to interfacial O sites results in downshift of p-band center of O sites that promote desorption of polysulfides and the cleavage of Li-S and S-S, accelerating the conversion kinetics of polysulfides. The designed composite cathode material delivers outstanding electrochemical performance in Li-S batteries, outperforming the recently reported similar cathodes. The concept could provide valuable insight into the design of other catalysts for Li-S batteries and beyond.