Abstract
Polymeric carbon nitride (PCN) has great potential for peroxydisulfate (PDS) activation but still challenge due to the sluggish electron-hole pair dissociation and tardy charge transfer dynamics. Herein, a novel PCN-based donor-acceptor conjugated polymer (PCN/4-MI D-A) is synthesized by copolymerization of urea and 4-methoxyphenyl isothiocyanate. The obtained PCN/4-MI D-A exhibited significantly improved activity on PDS activation for nitenpyram (NTP) degradation under visible light. As a result, PDS+PCN/4-MI_(75) shows the highest kinetic constants (0.115 min~(-1)), which is ～6.8 times as that of the pure PCN. Density functional theory (DFT) calculations indicated that 4-methoxyphenyl as an electron-donating group promotes the charge separation/transfer of PCN/4-MI D-A. In addition, the PCN/4-MI D-A is more conducive to the PDS adsorption at the position where the amino group linked with 4-MI. The PCN/4-MI D-A generated abundant electrons which were subsequently transferred to the PDS by tunneling effect. This study provides a new design concept for the highly efficient PDS activation by constructed PCN-based donor-acceptor conjugated polymers.
NSTL