Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and Health, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China.
School of Environment, Key Laboratory for Yellow River and Huaihe River Water Environment and Pollution Control, Henan Normal University, Xinxiang 453007, China.
J Hazard Mater. 2023 Oct 15;460:132401. doi: 10.1016/j.jhazmat.2023.132401. Epub 2023 Aug 24.
The peracetic acid (PAA)-activation process has attracted much attention in wastewater treatment. However, the low electron efficiency at the interface between heterogeneous catalysts and PAA has affected its practical application. For this study, we developed a carbon nitride hollow-nanotube catalysts with dispersed Cu(I) sites (Cu(I)-TCN) for the photocatalytic activation of PAA for antibiotics degradation. The obtained Cu(I)-TCN catalyst demonstrated an enhanced capacity for visible light harvesting along with increased charge transfer rates. Specifically, the developed Cu(I)-TCN/visible light/PAA system was able to completely remove antibiotics within 20 min, with a kinetic constant that was 25 times higher than a Cu(I)-TCN/visible light system, and 83 times higher than Cu(I)-TCN/PAA systems. Scavenging experiment and electron paramagnetic resonance (EPR) indicated that singlet oxygen was dominant reactive specie for sulfisoxazole (SIZ) removal. Besides, electrochemical tests and attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy verified that the electron transfer efficiency of PAA activation was promoted due to the formation of inner-sphere interactions between PAA and Cu(I)-TCN, resulting in the quick removal of antibiotics. Further, after exposure to visible light, the Cu(I)-TCN excited photogenerated electrons which supplemented the electrons consumed in the reaction and drove the valence cycle of Cu ions. Overall, this research offered novel insights into the non-radical pathway for heterogeneous visible light-driven advanced oxidation processes and their potential for practical wastewater remediation.
过氧乙酸（PAA）的激活过程在废水处理中受到了广泛关注。然而，异相催化剂与 PAA 界面处的低电子效率影响了其实际应用。在这项研究中，我们开发了一种具有分散的 Cu(I)位点的氮化碳中空纳米管催化剂（Cu(I)-TCN），用于光催化 PAA 激活以降解抗生素。所获得的 Cu(I)-TCN 催化剂表现出增强的可见光捕获能力以及增加的电荷转移速率。具体而言，所开发的 Cu(I)-TCN/可见光/PAA 系统能够在 20 分钟内完全去除抗生素，其动力学常数比 Cu(I)-TCN/可见光系统高 25 倍，比 Cu(I)-TCN/PAA 系统高 83 倍。清除实验和电子顺磁共振（EPR）表明，单线态氧是磺胺异恶唑（SIZ）去除的主要反应物质。此外，电化学测试和衰减全反射傅里叶变换红外（ATR-FTIR）光谱证实，由于 PAA 和 Cu(I)-TCN 之间形成内球相互作用，促进了 PAA 激活的电子转移效率，从而快速去除抗生素。此外，在暴露于可见光后，Cu(I)-TCN 激发的光生电子补充了反应中消耗的电子，并驱动 Cu 离子的价循环。总体而言，这项研究为非自由基途径的异相可见光驱动高级氧化过程及其在实际废水修复中的应用提供了新的见解。
