A 3D porous sulfur/graphene@g‐C₃N₄ (S/GCN) hybrid sponge, which can be directly applied as a free‐standing cathode for Li–S batteries, is realized via a microemulsion assisted assembly approach. In this strategy, the interior oil emulsion droplets serve as soft templates to form pores to accommodate sulfur and the hydrophilic GCN stacks around oil droplets to assemble into a crosslinked 3D network. Through this microemulsion encapsulation route, S/GCN cathodes with a sulfur loading as high as 82 wt% can be achieved. Furthermore, the enriched N‐sites in GCN macropores offer numerous adhesion sites for polysulfides, realizing a “physical‐chemical” dual‐confinement for polysulfides from diffusion. Moreover, the robust and highly porous 3D graphene frameworks render efficient electron/Li⁺ transport pathways for fast kinetics as well as good structure integrity. Consequently, in comparison to the conventional G‐sponge/Li₂S_n catholyte system, S/GCN delivers a higher specific capacity, superior high‐rate capability (612 mA h g⁻¹ at 10 C), and alleviated anode corrosion issues. Particularly, an energy density as high as 1493 W h kg⁻¹ (calculated on the total weight of the cathode) and an extremely low capacity fading rate of 0.017% per cycle over 800 cycles at 0.3 C are achieved.

中文翻译：

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微乳液辅助组装3D多孔S / Graphene @ g-C3N4混合海绵，作为高能量密度Li-S电池的自立阴极

一种3D多孔硫/石墨烯g C ₃ N ₄（S / GCN）混合海绵，可以通过微乳液辅助组装方法直接用作Li-S电池的独立式阴极。在这种策略中，内部油乳剂小滴充当软模板以形成孔以容纳硫，并且油滴周围的亲水性GCN堆叠会组装成交联的3D网络。通过这种微乳液包封途径，可以实现硫含量高达82重量％的S / GCN阴极。此外，GCN大孔中富集的N位点为多硫化物提供了许多粘附位点，从而实现了扩散过程中多硫化物的“物理化学”双重限制。此外，坚固且高度多孔的3D石墨烯骨架可提供有效的电子/锂⁺快速的动力学以及良好的结构完整性的运输途径。因此，与传统的G-ponge / Li ₂ S _n阴极电解液体系相比，S / GCN具有更高的比容量，更高的高倍率容量（在10 C时为612 mA hg ^-1），并减轻了阳极腐蚀问题。特别地，在0.3C下在800次循环中实现了高达1493W h kg ^-1的能量密度（以阴极的总重量计算）和极低的每循环0.017％的容量衰减率。