Synthesis of Ionic Vinylene‐Linked Covalent Organic Frameworks through Quaternization‐Activated Knoevenagel Condensation

We developed a simple approach to synthesizing ionic vinylene‐linked two‐dimensional covalent organic frameworks (COFs) through a quaternization‐promoted Knoevenagel condensation at three aromatic methyl carbon atoms ofN‐ethyl‐2,4,6‐trimethylpyridinium halide with multitopic aromatic aldehyde derivatives. The resultant COFs exhibited a honeycomb‐like structure with high crystallinity and surface areas as large as 1343 m2 g−1. The regular shape‐persistent nanochannels and the positively charged polymeric frameworks allowed the COFs to be uniformly composited with linear polyethylene oxide and lithium salt, displaying ionic conductivity as high as 2.72×10−3 S cm−1.