Effective Bidirectional Mott-Schottky Catalysts Derived from Spent LiFePO Cathodes for Robust Lithium-Sulfur Batteries.

It is deemed as a tough yet profound project to comprehensively cope with a range of detrimental problems of lithium-sulfur batteries (LSBs), mainly pertaining to the shuttle effect of lithium polysulfides (LiPSs) and sluggish sulfur conversion. Herein, a CoP-FeP@N-doped carbon (CoP-FeP@NC) Mott-Schottky catalyst is introduced to enable bidirectionally stimulated sulfur conversion. This catalyst is prepared by simple carbothermal reduction of spent LiFePO cathode and LiCoO. The experimental and theoretical calculation results indicate that thanks to unique surface/interface properties derived from the Mott-Schottky effect, full anchoring of LiPSs, mediated LiS nucleation/dissolution, and bidirectionally expedited "solid⇌liquid⇌solid" kinetics can be harvested. Consequently, the S/CoP-FeP@NC manifests high reversible capacity (1569.9 mAh g), superb rate response (808.9 mAh g at 3C), and stable cycling (a low decay rate of 0.06% within 600 cycles at 3C). Moreover, desirable capacity (5.35 mAh cm) and cycle stability are still available under high sulfur loadings (4-5 mg cm) and lean electrolyte (8 µL mg) conditions. Furthermore, the as-proposed universal synthetic route can be extended to the preparation of other catalysts such as MnP-FeP@NC from spent LiFePO and MnO. This work unlocks the potential of carbothermal reduction phosphating to synthesize bidirectional catalysts for robust LSBs.