Electrocatalytic conversion of polysulfides is an effective strategy to alleviate shuttle effects for Li-S batteries, but achieving the synergistic effects between strong adsorption and high catalytic activity with a single catalyst is still challenging. Herein, we report the rational balancing of strong adsorption and high catalytic activity on the tailored ZnO-ZnS/reduced graphene oxide (rGO) heterostructure to achieve significantly enhanced conversion of polysulfides. By integrating the merits of adsorptive ZnO, catalytic ZnS and conductive rGO, the ZnO-ZnS/rGO heterostructures could enable an unrestricted adsorption-diffusion-conversion of polysulfides. Moreover, by controlling the sulfurization degree, the ZnO-ZnS/rGO heterostructure with ZnO/ZnS ratio of 7:3 performs the optimized overall performance, indicative of a trade-off between adsorption and catalytic activity. When served as functional coatings onto the separators, the ZnO-ZnS/rGO heterostructures could greatly promote the redox kinetics and retrain the polysulfides shuttling. The pure sulfur cathode with the 7ZnO-3ZnS/rGO modified separator delivers a high initial specific capacity of 1186 mAh g⁻¹ at 0.5 ℃ and a low capacity fading of 0.06% per cycle over 500 cycles at 1 ℃. Even with high sulfur loading of 7.6 mg cm⁻², a high reversible specific capacity of 671 mAh g⁻¹ at 1 ℃ can still be retained. This work presents a rational method to tailor the heterostructure catalysts for boosting electrocatalytic conversion of polysulfides towards high-performance Li-S batteries.

多硫化物的电催化转化是减轻Li-S电池穿梭效应的有效策略，但用单一催化剂实现强吸附和高催化活性之间的协同效应仍然具有挑战性。在此，我们报告了在定制的 ZnO-ZnS/还原氧化石墨烯 (rGO) 异质结构上强吸附和高催化活性的合理平衡，以显着提高多硫化物的转化率。通过结合吸附 ZnO、催化 ZnS 和导电 rGO 的优点，ZnO-ZnS/rGO 异质结构可以实现多硫化物的无限制吸附-扩散-转化。此外，通过控制硫化程度，ZnO/ZnS 比为 7:3 的 ZnO-ZnS/rGO 异质结构实现了优化的整体性能，表明吸附和催化活性之间的权衡。当用作隔膜上的功能涂层时，ZnO-ZnS/rGO异质结构可以极大地促进氧化还原动力学并重新训练多硫化物穿梭。采用 7ZnO-3ZnS/rGO 改性隔膜的纯硫正极提供 1186 mAh g 的高初始比容量^{在 0.5 ℃ 时为-1}，在 1 ℃ 下 500 次循环后容量衰减低至每循环 0.06%。^{即使在 7.6 mg cm -2}的高硫负载下，1 ℃时仍可保持671 mAh g ^-1的高可逆比容量。这项工作提出了一种合理的方法来定制异质结构催化剂，以促进多硫化物向高性能锂硫电池的电催化转化。