Hierarchical sulfur-impregnated hydrogenated TiO2 mesoporous spheres comprising anatase nanosheets with highly exposed (001) facets for advanced Li-S batteries.

In this contribution, we purposefully designed hierarchical hydrogenated TiO2 spheres (HTSs) constructed from ultrathin anatase nanosheets with highly exposed (001) facets, and further utilized them as an efficient encapsulated host of sulfur species for advanced Li-S batteries (LSBs). Strikingly, the as-fabricated hybrid S/HTSs cathode exhibited high Coulombic efficiency (>94%), exceptional long cycling performance (capacity decay of ∼0.399% per cycle at 0.5 C), and large reversible discharge capacity (∼579 mAh g(-1) at 2.0 C) at high C rates, benefiting from better electronic conductivity, smaller charge transfer resistance and strong chemical bonding between [Formula: see text] and the reduced (001) facets of HTSs, according to experimental measurements and systematical theoretical calculations. More significantly, our in-depth insights into the mechanism involved in the hybrid S/HTSs could efficiently guide future design, optimization and synthesis of other metal oxide-based matrixes with specific exposed crystal facets for next-generation advanced LSBs.