Litcius/Paper detail

Synthesis of Rigid Stepladder Polymers <i>via</i> Scandium-Catalyzed Polyspiroannulation of Quinoline with Alkyne

Jingjing Shao, Lin Huang, Shao‐Jie Lou, Aya Ohno, Yoichi M. A. Yamada, Masayoshi Nishiura, Tetsuro Murahashi, Zhaomin Hou

2025Journal of the American Chemical Society11 citationsDOI

Abstract

Polymers with rigid three-dimensional architectures have attracted significant attention due to their high rigidity and intrinsic microporosity. Here, we report the synthesis of a new class of rigid stepladder polymers featuring unique spirodihydroquinoline skeletons. Under the catalysis of a half-sandwich scandium catalyst, quinoline compounds bearing both an aryl substituent (e.g., phenyl or naphthyl) and an alkynyl group (e.g., C≡CSiMe 3 ) selectively undergo dearomative polyspiroannulation between the quinoline skeleton and the alkyne unit via ortho -C–H activation of the aryl group. This reaction efficiently yields rigid stepladder polymers comprising a spirodihydroquinoline skeleton with a quaternary carbon stereocenter and an unprotected N–H group. Treatment of the N–H-containing polymers with an alkyl lithium reagent followed by methyl iodide leads to quantitative formation of the corresponding N -methylated polymers, which exhibit enhanced thermal stability and porosity compared to their N–H counterparts.

Topics & Concepts

ChemistryAlkyneQuinolineArylScandiumSubstituentCatalysisPolymer chemistryPolymerAlkylMedicinal chemistryOrganic chemistryCovalent Organic Framework ApplicationsMembrane Separation and Gas TransportOrganoboron and organosilicon chemistry