Microdroplet-Enabled Interfacial Electron Transfer Accelerates Schiff Base Condensation for Ultrafast Covalent Organic Framework Synthesis.

Authors

Zhendong Luo, Peng Jin, Junju Mu, Zilun Yu, Sihui Meng, Jianhan Wu, Xuke Chen, Xukai Zhou, Feng Wang

Published in

Journal of the American Chemical Society. Jun 17, 2026. Epub Jun 17, 2026.

Abstract

Imine-linked covalent organic frameworks (COFs) are attractive crystalline porous materials, yet their synthesis is kinetically limited by sluggish acid-catalyzed Schiff base condensation. Here we report a microdroplet-driven strategy that enables rapid and scalable COF formation via an unconventional interfacial pathway. Continuous ultrasonic nebulization of aqueous monomers affords crystalline imine-linked COFs within minutes at room temperature, without catalysts or organic solvents, achieving reaction rates orders of magnitude higher than batch synthesis. Mechanistic studies reveal the gas-liquid interface of microdroplets as an electronically active reaction zone, where interfacial electron transfer generates radical and anionic nitrogen species that trigger a nonclassical condensation mechanism. Interfacial enrichment, hydrogen-bond symmetry breaking, and strong electric fields cooperatively lower activation barriers and promote dehydration-driven framework growth. This general and scalable platform transforms the air-water interface into an active electronic reactor, establishing a new paradigm for framework synthesis and interfacial reaction acceleration.

PMID:
42310307
Bibliographic data and abstract were imported from PubMed on 18 Jun 2026.

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