Abundant defect-induced nonradiative recombination greatly
reduces
the charge separation efficiency in photocatalysts. Dielectric screening
of defects has been proven to be an effective strategy to improve
the charge separation efficiency; however, it has been rarely reported
in photocatalysis. Here, a developed calcium poly(heptazine imide)
(CaPHI) is utilized as a model photocatalyst to explore the dielectric
screening of defects. Through embedding potassium ions in CaPHI, the
dipole moment and polarity of the PHI structure are increased, thus
enhancing the dielectric constant and enabling the dielectric screening
of defects. In addition, compared to the original CaPHI, the optimized
Ca/KPHI exhibits a 79.3% reduction in defect capture cross-section,
and a decrease in the nonradiative recombination rate from 0.6224
to 0.1452 ns–1, thus achieving an apparent quantum
efficiency of 51.4% for H2 production at 420 nm. This proposed
dielectric screening strategy effectively addresses the issue of slow
carrier transport and separation caused by defect-induced nonradiative
recombination in photocatalysts.