Novel Donor-Acceptor Structured Ionic Organic Framework/Porous Carbon Nitride for Efficient Photocatalysis Imine Synthesis

Abstract

The development of efficient photocatalysts for imine synthesis is challenging due to C=N bond instability and limitations of thermal methods. Herein, we designed π-conjugated monomers with donor-acceptor (D-A) features from ionic liquid precursors and, for the first time, constructed ionic organic frameworks (IOFs). Coupling IOFs with porous carbon nitride (PCN) yielded IOFx/PCNy composites. IOF5/PCN5 achieved 98% conversion and 99% selectivity in light-driven benzylamine oxidative coupling. Combined mechanistic and photoelectrochemical studies revealed that imidazolium cations and D-A units synergistically promoted charge transfer and suppressed recombination. Furthermore, the composites elevated the conduction band potential of PCN without altering its bandgap, enhancing oxidation capability. These synergistic effects explain the superior activity. This work pioneers the application of IOFs in photocatalysis, establishing a tailored polymeric framework designed for precise functional control and enhanced photocatalytic performance, which highlights the potential of donor-acceptor design in ionic materials and offers a novel strategy for advanced photocatalyst development