Boosting the Quantum Efficiency of Ionic Carbon Nitrides in Photocatalytic H2O2 Evolution via Controllable n → π* Electronic Transition Activation
Abstract
Hydrogen peroxide (H2O2) is a crucial chemical used in numerous industrial applications, yet its manufacturing relies on the energy‐demanding anthraquinone process. Solar‐driven synthesis of H2O2 is gaining traction as a promising research area, providing a sustainable method for its production. Herein, a controllable activation of n → π* electronic transition is presented to boost the photocatalytic H2O2 evolution in ionic carbon nitrides. This enhancement is achieved through the simultaneous introduction of structural distortions and defect sites (─C ≡ N groups and N vacancies) into the KPHI framework. The optimal catalyst (2%Ox‐KPHI) reached an apparent quantum yield of 41% at 410 nm without the need for any cocatalysts, outperforming most previously reported carbon nitride‐based photocatalysts. Extensive experimental characterizations and theoretical calculations confirm that a corrugated configuration and the presence of defects significantly broaden the light absorption profile, improve carrier separation and migration, promote O2 adsorption, and lower the energy barriers for H2O2 desorption. Transient absorption spectroscopy indicates that the enhanced photocatalytic performance of 2%Ox‐KPHI is largely attributed to the preferential migration of electrons at defect sites over extended timescales, following the diffusion of geminate carriers across the PHI sheets.
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