[Ph3C][B(C6F5)4]: A Highly Efficient Metal‐Free Single‐Component Initiator for the Helical‐Sense‐Selective Cationic Copolymerization of Chiral Aryl Isocyanides and Achiral Aryl Isocyanides

: Commercially available [Ph3 C][B(C6 F5 )4 ] served as a highly efficient metal-free and single-component initiator not only for the carbocationic polymerization of polar and bulky aryl isocyanides with extremely high activity up to 1.2×107  g of polymer/(molcat.  h), but also for the helical-sense-selective polymerization of chiral aryl isocyanides and copolymerization with achiral aryl isocyanides to afford high-molecular-weight functional poly(aryl isocyanide)s with good solubility as well as AIE characteristics and/or a single-handed helical conformation.