Lithium-chalcogen batteries, including lithium-sulfur (Li-S) and lithium selenium (Li-Se) systems, have been recognized as promising candidates for high energy electrical storage solution. The key challenge for lithium-chalcogen systems is to increase the chalcogen content in the system without sacrificing performance in order to compete with Li-ion batteries. Here we report a rationally designed hierarchical porous carbon (SPC) electrode architectures with maximum micro-, meso- and macro-level porosities as the conductive framework for the lithium-chalcogen batteries. The hierarchical electrode architectures enable high mass loading of the active cathode materials, encapsulation of both the small and long chain chalcogenide species, reduced SEI reaction, and efficient mass transport in the electrolyte. The ideal cathode architecture to allow a maximum conversion reaction mechanism is identified for stable cycling. Cell level calculations suggests that the hierarchical electrode architectures have the potential to increase the specific energy to more than 350 Wh kg⁻¹, much higher than what can be achieved using the materials and parameters reported in the literature.

锂硫族电池，包括锂硫（Li-S）和锂硒（Li-Se）系统，已被公认为是高能蓄电解决方案的有希望的候选者。锂硫属元素体系的关键挑战是在不牺牲性能的情况下增加体系中的硫属元素含量，以便与锂离子电池竞争。在这里，我们报告了合理设计的分层多孔碳（SPC）电极体系结构，具有最大的微观，中观和宏观孔隙率，作为锂硫属元素电池的导电框架。分层的电极架构可实现活性阴极材料的高质量负载，小链和长链硫族化物物种的封装，减少的SEI反应以及在电解质中的有效质量传输。确定了允许最大转化反应机理的理想阴极结构，以实现稳定的循环。单元级计算表明，分层电极结构有可能将比能提高到350 Wh kg以上^-1，比使用文献中报道的材料和参数所能达到的要高得多。