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The serious shuttle effect, sluggish reduction kinetics of polysulfides and the difficult oxidation reaction of Li 2 S have hindered LiS battery practical application. Herein, a 3D hierarchical structure composed of NiMoO 4 nanosheets in situ anchored on NS doped carbon clothes (NiMoO 4 @NSCC) as the free-standing host is creatively designed and constructed for LiS battery. Dual transitional metal oxide (NiMoO 4 ) increases the electrons density near the Fermi level due to the contribution of the incorporating molybdenum (Mo), leading to the smaller bandgap, and thus stronger metallic properties compared with NiO. Furthermore, as a bidirectional catalyst, NiMoO 4 is proposed to facilitate reductions of polysulfides through lengthening the SS bond distance of Li 2 S 4 and reducing the free energy of polysulfides conversion, meanwhile promote critical oxidation of insulative discharge product (Li 2 S) via lengthening LiS bond distance of Li 2 S and decreasing Li 2 S decomposition barrier. Therefore, after loading sulfur (2 mg cm −2 ), NiMoO 4 @NSCC/S as the self-supporting cathode for the LiS battery exhibits impressive long cycle stability. This study proposes a concept of a bidirectional catalyst with dual metal oxides, which would supply a novel vision to construct the high-performance LiS battery.

The polysulfide shuttle effect is one of the most important problems hindering the commercial application of lithium−sulfur batteries (LSBs). In order to solve the above problem and promote LSBs commercialization, herein a holistic design strategy on the molybdenum disulfide-coated nitrogen-doped mesoporous carbon sphere/sulfur (NMCS@MoS 2 /S) composite cathode and carbon nanotube/chitosan modified separator (CNT/CH) is proposed. In the holistic design, the NMCS@MoS 2 plays a role in the host of sulfur and the lithium polysulfides (LiPSs) adsorbent; the CNT/CH modified separator also has an inestimable role in promoting lithium ion transport and chemical adsorption of LiPSs. The results show that the LSBs with the NMCS@MoS 2 /S-CNT/CH release a high reversible capacity of 827 mAh g −1 with a high capacity retention of 92.4% at 0.5 C after 200 cycles. The delicate design exhibits apparently excellent electrochemical performance and provides an exciting strategy for solving the shuttle effect of LiPSs and boosting industrialization of LSBs.

The commercialization of lithium‐sulfur (Li‐S) batteries is greatly hindered due to serious capacity fading caused by the polysulfide shuttling effect. Optimizing the structural configuration, enhancing reaction kinetics of the sulfur cathode, and increasing areal sulfur loading are of great significance for promoting the commercial applications of Li‐S batteries. Herein, the multifunctional polysulfide scavengers based on nitrogen, sulfur co‐doped carbon cloth (DCC), which is supported by flower‐like MoS2 (1T‐2H) decorated with BaMn0.9Mg0.1O3 perovskite particle (PrNP) and carbon nanotubes (CNTs), namely, DCC@MoS2/PrNP/CNTs, are delicately designed and synthesized. The physical confinement, chemical coupling, and catalysis conversion for active sulfur are achieved simultaneously in this polysulfide motif. Due to these merits, the as‐fabricated self‐supported DCC@MoS2/PrNP/CNTs/S manifests an excellent reversible areal capacity of 4.75 mAh cm−2 with an ultrahigh sulfur loading of 5.2 mg cm−2 at the 50th cycle. The outstanding cycling stability is obtained upon 800 cycles with a large reversible capacity of 871 mAh g−1 and a negligible fading rate of 0.02% per cycle at a rate of 1.0 C, suggesting its promising prospects for the commercial success of high‐performance Li‐S batteries toward flexible electronic devices and energy storage equipment.

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