Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-03-07 , DOI: 10.1016/j.cej.2022.135667 Yingnan Sun 1, 2 , Dandan Wang 3 , Yongfa Zhu 1
Perylene diimide (PDI) was subjected to terminal substitution with nicotinic acid (NA) to prepare a unique, bi-planar, π-π conjugated, ultrathin, porous supramolecular photocatalyst (hp-PDi-NA). The photocatalytic activity of hp-PDI-NA for phenol degradation under visible light was approximately 3.5 times that of nano-PDI. hp-PDI-NA exhibited prominent mineralization ability, inducing almost complete mineralization of phenol. The hp-PDI-NA supramolecular photocatalyst was highly stable and maintained 98% of its initial activity after five experimental cycles (35 h). hp-PDI-NA also showed strong degradation and mineralization ability for model antibiotics (oxytetracycline (OTC)), and hormones (ethinylestradiol (EE)). The small steric hindrance, double π-π conjugation effect, and existence of layered pores with a thickness of less than 1 nm shortened the distance between the supramolecular layers and effectively improved the transmission and separation of photogenerated carriers. Combined with theoretical calculations, a mechanism explaining the possible influence of the bi-planar structure on the photocatalytic activity was proposed. The results demonstrate that terminal substitution with aromatic compounds, instead of aliphatic compounds, is an important strategy for improving the performance of PDI supramolecular photocatalysts.
中文翻译:
具有独特双平面π-π共轭的苝二亚胺超分子光催化剂深度降解污染物
用烟酸(NA)对苝二亚胺(PDI)进行末端取代,制备出独特的双平面π-π共轭超薄多孔超分子光催化剂(hp -PDi-NA)。hp -PDI-NA在可见光下对苯酚降解的光催化活性约为nano-PDI的3.5倍。hp -PDI-NA表现出显着的矿化能力,使苯酚几乎完全矿化。hp -PDI-NA超分子光催化剂高度稳定,在五个实验循环(35 小时)后保持其初始活性的 98%。生命值-PDI-NA对模型抗生素(土霉素(OTC))和激素(炔雌醇(EE))也表现出很强的降解和矿化能力。较小的空间位阻、双π-π共轭效应以及厚度小于1 nm的层状孔的存在缩短了超分子层之间的距离,有效改善了光生载流子的传输和分离。结合理论计算,提出了解释双平面结构对光催化活性可能影响的机理。结果表明,用芳香族化合物代替脂肪族化合物进行末端取代是提高PDI超分子光催化剂性能的重要策略。