A carbon host capable of effective and uniform sulfur loading is the key for lithium–sulfur batteries (LSBs). Despite the application of porous carbon materials of various morphologies, the carbon hosts capable of uniformly impregnating highly active sulfur is still challenging. To address this issue, we demonstrate a hierarchical pore-structured CNT particle host containing spherical macropores of several hundred nanometers. The macropore CNT particles (M-CNTPs) are prepared by drying the aerosol droplets in which CNTs and polymer particles are dispersed. The spherical macropore greatly improves the penetration of sulfur into the carbon host in the melt diffusion of sulfur. In addition, the formation of macropores greatly develops the volume of the micropore between CNT strands. As a result, we uniformly impregnate 70 wt % sulfur without sulfur residue. The S-M-CNTP cathode shows a highly reversible capacity of 1343 mA h g^–1 at a current density of 0.2 C even at a high sulfur content of 70 wt %. Upon a 10-fold current density increase, a high capacity retention of 74% is observed. These cathodes have a higher sulfur content than those of conventional CNT hosts but nevertheless exhibit excellent performance. Our CNTPs and pore control technology will advance the commercialization of CNT hosts for LSBs.

中文翻译：

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具有超高硫负荷的球形大孔碳纳米管颗粒，用于锂-硫电池阴极

能够有效且均匀地加载硫的碳载体是锂硫电池（LSB）的关键。尽管应用了各种形态的多孔碳材料，但是能够均匀地浸渍高活性硫的碳主体仍然具有挑战性。为了解决这个问题，我们演示了包含数百纳米球形大孔的分层孔结构的CNT颗粒主体。通过干燥分散有CNT和聚合物颗粒的气雾剂液滴来制备大孔CNT颗粒（M-CNTP）。球形大孔极大地提高了硫在熔体扩散过程中硫向碳主体的渗透。另外，大孔的形成极大地发展了CNT链之间的微孔的体积。因此，我们均匀地浸渍了70 wt％的硫，而没有硫残留物。SM-CNTP阴极显示出1343 mA hg的高度可逆容量即使在70 wt％的高硫含量下，电流密度为0.2 C时^仍为–1。当电流密度增加10倍时，观察到74％的高容量保持率。这些阴极的硫含量高于常规CNT主体的硫含量，但仍具有出色的性能。我们的CNTP和孔控制技术将推动用于LSB的CNT主体的商业化。