The practical applications of lithium-sulfur (Li-S) battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode. One of the effective solutions deals with concurrent management of both electrodes. Nevertheless, this direction remains in a nascent stage due to a lack of material selection and mechanism exploration. Herein, we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene (BNG) particulated architectures, which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries. Benefiting from the “sulfiphilic” and “lithiophilic” features, the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth. Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level. This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.

锂硫（Li-S）电池的实际应用受到阴极严重的多硫化物穿梭和阳极锂枝晶生长的严重阻碍。有效的解决方案之一是同时管理两个电极。然而，由于缺乏材料选择和机制探索，该方向仍处于起步阶段。在此，我们设计了一种温度介导的直接化学气相沉积策略，以实现三维硼/氮双掺杂石墨烯 (BNG) 颗粒结构的可控合成，该结构用作两种材料的轻量化和多功能介质。锂硫电池中的电极。得益于“亲硫”和“亲锂”的特性，BNG 改性隔膜不仅能够提高多硫化物转化的动力学以减轻穿梭效应，而且还能赋予均匀的锂沉积以抑制枝晶生长。结合电动试验的理论计算和操作拉曼分析在分子水平上进一步阐明了 BNG 有利的硫和锂电化学。这项工作通过石墨烯材料的可控合成提供了对介体设计的直接洞察，以解决锂硫电池的基本挑战。