Search

The serious shuttle effect, sluggish reduction kinetics of polysulfides and the difficult oxidation reaction of Li2S have hindered LiS battery practical application. Herein, a 3D hierarchical structure composed of NiMoO4 nanosheets in situ anchored on NS doped carbon clothes (NiMoO4@NSCC) as the free‐standing host is creatively designed and constructed for LiS battery. Dual transitional metal oxide (NiMoO4) 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, NiMoO4 is proposed to facilitate reductions of polysulfides through lengthening the SS bond distance of Li2S4 and reducing the free energy of polysulfides conversion, meanwhile promote critical oxidation of insulative discharge product (Li2S) via lengthening LiS bond distance of Li2S and decreasing Li2S decomposition barrier. Therefore, after loading sulfur (2 mg cm−2), NiMoO4@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. [ABSTRACT FROM AUTHOR]

• VC 0.75 /Co-CoO was applied as a host in Li-S battery for the first time. • The catalytic activity towards polysulfides is regulated. • The bifunctional catalytic effect of VC 0.75 /Co-CoO is analyzed. The shuttle effect and sluggish redox kinetics of lithium polysulfides lead to a short lifespan and poor rate capability of lithium-sulfur (Li-S) batteries. Introducing electrocatalysts into sulfur host materials has been deemed a promising strategy to overcome these issues in Li-S batteries. Herein, an efficient catalytic sulfur host material (i.e., VC 0.75 /Co-CoO) has been fabricated by simply pyrolyzing the electrospun vanadium and cobalt salt-based polymer fibers. Electrochemical measurements demonstrated that the as-formed heterostructure of Co-CoO with VC 0.75 evidently strengthens the redox kinetics of polysulfides due to the enhanced adsorption ability to polysulfides and adjusts the electronic structure of heterostructure via the introduction of VC 0.75. Further theoretical computation discloses that Co-CoO mainly plays the role in stretching the S S bond in polysulfides to facilitate the reduction of polysulfide, extending the Li-S bond in Li 2 S and reducing energy barriers of Li 2 S decomposition to promote the oxidation process of Li 2 S. Accordingly, the collaboration of Co-CoO and VC 0.75 synergetically facilitates the redox kinetics of polysulfides, prolonging the lifespan of Li-S batteries. Impressively, VC 0.75 /Co-CoO composites endow Li-S batteries with a discharge capacity decay rate as low as 0.02 % per cycle at the current density of 0.2 C. The specific capacity reaches 626 mAh/g at the high current density of 1.0 C even after 450 cycles. This work sheds light on a facile methodology for improving the catalytic activity of sulfur host materials in Li-S batteries. [ABSTRACT FROM AUTHOR]