Rational design of dual sites induced local electron rearrangement for enhanced photocatalytic oxygen activation

Abstract

Efficiently activated molecular oxygen (O2) is considered a promising technique for the removal of antibiotics. However, how to effectively regulate electrons distribution to promote O2 activation remains a challenge at present. In this study, phosphorus and sodium co-doped carbon nitride (PNaCN) were designed to rearrange the electrons distribution to activate O2 for the degradation of tetracycline. The generation of •O2− was innovatively observed via in-situ O2 fitting Fourier transform infrared (FTIR) spectroscopy, demonstrating the outstanding O2 activation ability of PNa5. Density functional theory (DFT) further confirmed that the rational co-doping led to the rearrangement of local electrons, resulting in electron-rich Na sites and electron-deficient P sites. These sites exhibited greater susceptibility to O2 adsorption and charge transfer. Besides, the degradation rate of tetracycline was increased by 2.44 times using co-doped CN. This study provides a new inspiration for enhancing O2 activation by inducing electrons rearrangement.