Biotemplating Growth of Nepenthes-like N-Doped Graphene as a Bifunctional Polysulfide Scavenger for Li–S Batteries

The practical application of lithium–sulfur (Li–S) batteries is hindered by their poor cycling stabilities that primarily stem from the "shuttle" of dissolved lithium polysulfides. Here, we develop a nepenthes-like N-doped hierarchical graphene (NHG)-based separator to realize an efficient polysulfide scavenger for Li–S batteries. The 3D textural porous NHG architectures are realized by our designed biotemplating chemical vapor deposition (CVD) approach via the employment of naturally abundant diatomite as the growth substrate. Benefiting from the high surface area, devious inner-channel structure, and abundant nitrogen doping of CVD-grown NHG frameworks, the derived separator favorably synergizes bifunctionality of physical confinement and chemical immobilization toward polysulfides, accompanied by smooth lithium ion diffusions. Accordingly, the batteries with the NHG-based separator delivers an initial capacity of 868 mAh g–1 with an average capacity decay of only 0.067% per cycle at 2 C for 800 cycles. A capacity of 805 mAh g–1 can further be achieved at a high sulfur loading of ∼7.2 mg cm–2. The present study demonstrates the potential in constructing high-energy and long-life Li–S batteries upon separator modification.