Rational design of donor-acceptor conjugated polymers with high performance on peroxydisulfate activation for pollutants degradation

• Main Authors: Che, Huinan, Wang, Peifang, Chen, Juan, Gao, Xin, Liu, Bin, Ao, Yanhui
• Other Authors: School of Chemistry, Chemical Engineering and Biotechnology
• Format: Article
• Language: English
• Published: 2023
• Subjects: Engineering::Chemical engineering; Peroxydisulfate; Polymeric Carbon Nitride
• Online Access: https://hdl.handle.net/10356/172396
• Institution: Nanyang Technological University

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-MI75 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.