Covalent Triazine Frameworks Incorporating Charged Polypyrrole Channels for High-Performance Lithium–Sulfur Batteries

Organosulfur polymers have emerged as promising electrode materials for lithium–sulfur (Li–S) batteries, mainly because of their ability to incorporate and stabilize high sulfur content. The low ionic and electronic conductivity of these polymers, however, limit their cycling performance at high active mass loadings. Moreover, Li–polysulfide (Li–PS) shuttling, a fatal phenomenon in the cyclability of Li–S batteries, can be mitigated via the entrapment of Li–PS by utilizing various supramolecular interactions. Herein, we report a new approach that incorporates one-dimensional charged polypyrrole into a two-dimensional covalent triazine framework (cPpy-S-CTF) synthesized in the presence of elemental sulfur. The cPpy-S-CTF enabled sulfur loadings up to 83 wt %, thanks to the perfluoroaryl-elemental sulfur SN Ar chemistry. Notably, the addition of charged polypyrrole, cPpy, triggered a 3D na…