Despite outstanding theoretical energy density (2600
Wh kg–1) and low cost of lithium–sulfur (Li–S)
batteries, their practical application is seriously hindered by inferior
cycle performance and low Coulombic efficiency due to the “shuttle
effect” of lithium polysulfides (LiPSs). Herein, we proposed
a strategy that combines TiO–TiO2 heterostructure
materials (H-TiO
x
, x =
1, 2) and conductive polypyrrole (PPy) to form a multifunctional sulfur
host. Initially, the TiO–TiO2 heterostructure can
enhance the redox reaction kinetics of sulfur species and improve
the conductivity of sulfur cathode together with the PPy coating layer.
Moreover, the defect-abundant H-TiO
x
matrices
can trap LiPSs by the formation of Ti–S bond via the Lewis
acid–base interaction. Furthermore, the PPy coating can physically
hinder the diffusion of LiPSs, as well as chemically adsorb LiPSs
by the polar–polar mechanism. Benefiting from the synergistic
effect of H-TiO
x
and PPy layer, the novel
cathode delivered high specific capacities at different current rates
(1130, 990, 932, 862, and 726 mAh g–1 at 0.1, 0.2,
0.3, 0.5, and 1C, respectively) and an ultralow capacity decay of
0.0406% per cycle after 1000 cycles at 1C. This work can not only
indicate effectiveness of employing H-TiO
x
materials to realize the LiPSs immobilization but also shed light
on the feasibility of combining different materials to achieve the
multifunctional sulfur hosts for advanced Li–S batteries.