Lithium–sulfur (Li–S) batteries are recognized as promising candidates for next‐generation electrochemical energy storage systems owing to their high energy density and cost‐effective raw materials. However, the sluggish multielectron sulfur redox reactions are the root cause of most of the issues for Li–S batteries. Herein, a high‐efficiency CoSe electrocatalyst with hierarchical porous nanopolyhedron architecture (CS@HPP) derived from a metal–organic framework is presented as the sulfur host for Li–S batteries. The CS@HPP with high crystal quality and abundant reaction active sites can catalytically accelerate capture/diffusion of polysulfides and precipitation/decomposition of Li₂S. Thus, the CS@HPP sulfur cathode exhibits an excellent capacity of 1634.9 mAh g⁻¹, high rate performance, and a long cycle life with a low capacity decay of 0.04% per cycle over 1200 cycles. CoSe nanopolyhedrons are further fabricated on a carbon cloth framework (CC@CS@HPP) to unfold the electrocatalytic activity by its high electrical conductivity and large surface area. A freestanding CC@CS@HPP sulfur cathode with sulfur loading of 8.1 mg cm⁻² delivers a high areal capacity of 8.1 mAh cm⁻² under a lean electrolyte. This work will enlighten the rational design of structure–catalysis engineering of transition‐metal‐based nanomaterials for diverse applications.

中文翻译：

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具有分层多孔多面体纳米结构的高效CoSe电催化剂，可加速Li-S电池中多硫化物的转化。

锂硫（Li–S）电池因其高能量密度和具有成本效益的原材料而被公认为是下一代电化学储能系统的有希望的候选者。但是，缓慢的多电子硫氧化还原反应是Li-S电池大多数问题的根本原因。本文中，一种由金属-有机骨架衍生的具有分层多孔纳米多面体结构（CS @ HPP）的高效CoSe电催化剂被用作Li-S电池的硫主体。具有高晶体质量和丰富的反应活性位点的CS @ HPP可以催化加速多硫化物的捕获/扩散和Li ₂ S的沉淀/分解。因此，CS @ HPP硫阴极具有1634.9 mAh g ^-1的出色容量。，高倍率性能和长循环寿命，在1200个循环内每个循环的容量衰减低至0.04％。CoSe纳米多面体可在碳布骨架（CC @ CS @ HPP）上进一步制造，以其高电导率和大表面积展现其电催化活性。独立的CC @ CS @ HPP硫负载量为8.1 mg cm ^-2的CC @ CS @ HPP硫阴极在贫电解质下可提供8.1 mAh cm ^-2的高面积容量。这项工作将启发过渡金属基纳米材料用于各种应用的结构催化工程的合理设计。