<p>Polyaromatic materials, characterized by extended C–C/C = C conjugation, hold transformative potential for next‑generation plastic electronics. Herein, we present a click-like C = C bond-forming Aldol polycondensation that proceeds with exceptional efficiency and operational simplicity in air. Central to this finding is an enolate-mediated mechanism within a dual-catalytic process. Strategic control of adjacent heteroatom and ring geometry precisely modulates the proton transfer and the energy spans in the enol/enamine tautomerization pathways, thus the reactivity of ketone and imide monomers. This approach establishes both a design roadmap and a versatile tool box for tailored functionality. Notably, the in situ-generated acetic acid increases reactant oxidation potential enables air-tolerant operation, unlike conventional metal-catalyzed C–C couplings requiring oxygen-free conditions. This methodology facilitates rapid (typically within 30 min), modular assembly of multidimensional conjugated polymers, offering transformative potential for emerging plastic electronics and beyond.</p>

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Click-like Aldol Polycondensation in air for plastic electronics and beyond

  • Hongru Chen,
  • Hongyuan Fu,
  • Xiaofan Shi,
  • Shichao Wu,
  • Pinyu Chen,
  • Zhengkai Li,
  • Ming Zhang,
  • Mingyang Cui,
  • Fanchang Meng,
  • Shixin Meng,
  • Lingwei Xue,
  • Yuze Lin,
  • Zitong Liu,
  • Xugang Guo,
  • Ming Lei,
  • Zhi-Guo Zhang,
  • Yongfang Li

摘要

Polyaromatic materials, characterized by extended C–C/C = C conjugation, hold transformative potential for next‑generation plastic electronics. Herein, we present a click-like C = C bond-forming Aldol polycondensation that proceeds with exceptional efficiency and operational simplicity in air. Central to this finding is an enolate-mediated mechanism within a dual-catalytic process. Strategic control of adjacent heteroatom and ring geometry precisely modulates the proton transfer and the energy spans in the enol/enamine tautomerization pathways, thus the reactivity of ketone and imide monomers. This approach establishes both a design roadmap and a versatile tool box for tailored functionality. Notably, the in situ-generated acetic acid increases reactant oxidation potential enables air-tolerant operation, unlike conventional metal-catalyzed C–C couplings requiring oxygen-free conditions. This methodology facilitates rapid (typically within 30 min), modular assembly of multidimensional conjugated polymers, offering transformative potential for emerging plastic electronics and beyond.