Carbonyl heterocycle modified mesoporous carbon nitride in photocatalytic peroxydisulfate activation for enhanced ciprofloxacin removal: Performance and mechanism

过氧二硫酸盐 氮化碳 光化学 密度泛函理论 光催化 过硫酸盐 化学 石墨氮化碳 电子转移 介孔材料 材料科学 催化作用 计算化学 有机化学
作者
Kaijie Xu,Kangping Cui,Minshu Cui,Xueyan Liu,Xing Chen
出处
期刊:Journal of Hazardous Materials [Elsevier BV]
卷期号:444: 130412-130412 被引量:25
标识
DOI:10.1016/j.jhazmat.2022.130412
摘要

Polymer carbon nitride is considered to be a promising photocatalyst with broad application prospects in water treatment. However, the defects of pristine polymer carbon nitride (PCN), such as small specific surface area, fast photogenerated electron-hole recombination, and low mass transfer efficiency, limit its photocatalytic activity. In this work, by introducing 2-thiouracil into the precursor, a carbonyl heterocycle-containing mesoporous carbon nitride photocatalyst (TCN) was successfully obtained with significantly enhanced peroxydisulfate (PDS) photocatalytic activity. In this study, the modulation mechanism of carbonyl heterocycle introduction on surface electronic structure and the band structure were fully discussed by means of a combination of experiments and theoretical calculations. The carbonyl and vicinal carbon-modified heterocycles dominated the electrons, while the adjacent heptazine ring dominated the holes. The photogenerated electron-hole pair recombination efficiency and the electron transition energy barrier were greatly reduced. According to the findings of density functional theory (DFT) calculations, the introduction of carbonyl and vicinal C modulated the electronic structure of catalyst, enhanced the adsorption of PDS at the carbonyl ortho N site, which promoted the electronic interaction between TCN and PDS molecules. Experiments showed that the free radical pathway and non-radical pathway coexisted in TCN/PDS/Vis system. The reactive oxygen species were mainly derived from PDS molecules. DFT calculations provided a more comprehensive theoretical basis for the experimental results. This study provided a fresh perspective on the rational design of carbon nitride-based catalysts and the reaction mechanism of persulfate advanced oxidation systems.
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