Abstract
Porous organic polymers (POPs) have become a class of promising photocatalytic materials for solar water splitting due to their high structural adjustability, multiple active sites and high stability against water corrosion. However, because of the complex transfer process involved and the large overpotential required for oxygen evolution reaction (OER), the studies about POP type semiconductor photocatalysts for the efficient photocatalytic OER are very few. Here, we design and prepare a novel POP type photocatalyst 4Clper-POPs constructed by chlorine-modified peryleneimide and aromatic aldehyde that can significantly improve the photocatalytic OER activity. The band gap of as-synthesized 4Clper-POPs is 1.28 eV, indicating that they possess a wide light absorption range extended to the near-infrared region. Moreover, 4Clper-POPs exhibit a large oxidation potential to drive the photocatalytic OER. More importantly, combining the results of experiments and the first-principles calculations, under the condition of AgNO3 as the electronic sacrificial agent, it can be obtained that the chlorine element in the 4Clper-POPs can effectively accumulate AgNO3 and the reduced Ag nanoparticles (NPs), facilitating the rapid transport of electrons. Under visible light, 4Clper-POPs exhibit the highest average O2 evolution efficiency (714.17 μmol g-1h−1) with 5 wt% Co2+ loaded among all the reported POP materials used for the OER. Our findings provide design ideas of POP type semiconductor photocatalysts for the efficient OER.
Published Version
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