Photocatalytic
technique is regarded as the cleanest approach for
producing H2O2. Herein, two kinds of novel polyimide
COFs decorated with CQDs (namely, MPa-COFs/CQDs and MNd-COFs/CQDs)
were constructed by using the one-pot hydrothermal method. Due to
the electron donor role of CQDs, the recombination of photoinduced
electrons and holes was suppressed after the combination of polyimide
COFs with CQDs. Importantly, the introduction of CQDs not only boosted
the absorbing ability of polyimide COFs toward visible light but also
reduced the impedance and improved the charge transfer efficiency.
After CQDs were embedded into polyimide COFs, the surface hydrophilicity
of catalysts was significantly improved, which provided convenience
for the water oxidation reaction. Benefiting from the electron donor–acceptor
interaction between polyimide COFs and CQDs, a step-by-step two-electron
oxygen reduction reaction over polyimide COFs was enhanced. More interestingly,
the embedding of CQDs can create a direct two-electron water oxidation
reaction pathway, which played an important role in photocatalytic
H2O2 generation. Meanwhile, H+ generated
from water oxidation can also be used for the reduction of oxygen
to form H2O2. Under the synergistic effects
of water oxidation and oxygen reduction, as-prepared MPa-COFs/CQDs-2
displayed excellent performance in photocatalytic H2O2 generation, and its yield was as high as 540 μmol/g
within 60 min. In short, the current work shared an effective strategy
to improve the performance of polyimide COFs in photocatalytic H2O2 production.