Rational design of a well-aligned metal–organic framework nanopillar array for superior lithium-sulfur batteries

The polysulfide shuttle and the overgrowth of dendrites significantly challenge the large-scale promotion of lithium-sulfur (Li-S) batteries. Herein, a multifunctional Ni-based metal–organic framework-74 (Ni-MOF-74) nanopillar array supported on carbon nanotube (CNT) film is proposed for addressing these issues, simultaneously serving as the cathodic interlayer and anode host. For the polysulfide shuttle, the proposed interlayer possesses the adsorption and sieving effect of loose upper part and dense root for the MOF nanopillar array towards polysulfides, respectively, which also accelerates the redox kinetics by the catalytic Ni centers. For the other difficulty, the porous and expandable CNT film stores Li metal and deals with the anode volumetric expansion, while the MOF nanopillar array enables a uniform Li-ion distribution to avoid dendrite growth with the functions of its lithiophilic sites and ordered channels. Accordingly, Li-S full battery with the MOF-based interlayer and self-supporting anode exhibits a high capacity of 741 mAh g−1 and a persistent cyclability with an ultralow decay of 0.028 % per cycle over 1000 cycles at 5C. In addition, outstanding rate and cycle performances are still acquired at enhanced sulfur loadings with lean electrolyte.