Sun Siyu, Hu Youyou, Xu Mengshan, Cheng Fan, Zhang Hui, Li Zhengkui
State Key Laboratory of Pollution Control and Resource Reuse, Nanjing University, Nanjing 210023, China; School of the Environment, Nanjing University, Nanjing 210023, China.
State Key Laboratory of Pollution Control and Resource Reuse, Nanjing University, Nanjing 210023, China; School of the Environment, Nanjing University, Nanjing 210023, China.
J Hazard Mater. 2022 Feb 15;424(Pt C):127698. doi: 10.1016/j.jhazmat.2021.127698. Epub 2021 Nov 8.
Metal-organic frameworks have been widely used as photocatalytic materials. In this paper, a novel photocatalyst HSO-MIL-53(Fe) with acidity regulating groups was successfully synthesized by the solvothermal method and applied to remove carbamazepine (CBZ) and ibuprofen (IBP). The photodegradation efficiency of vis/HO/HSO-MIL-53(Fe) can reach 100% when the pH value is 8 or 9. The free radical capture experiment and electron paramagnetic resonance analysis proved that hole (h), hydroxide radical (·OH), singlet oxygen (O), and superoxide Radical (·O) are the main active species for pollutants degradation. In the vis/HO/HSO-MIL-53(Fe) system, the high pollutant degradation efficiency under alkaline conditions was attributed to two factors: (1) the acidity adjusting group -HSO adjusts the pH value of the whole system, which is beneficial to the photo-Fenton process. (2) The photogenerated electrons of HSO-MIL-53(Fe) can be captured by Fe (III), HO and O to accelerate the reduction of Fe (III) and generate ·OH, O, and ·O. Besides, HO can also be activated by Fe (II) and Fe (III). The above processes synergistically improved the photocatalytic efficiency. Based on liquid chromatography-mass spectrometry (LC-MS) analysis, the possible degradation pathways of the two pollutants were proposed.
金属有机框架材料已被广泛用作光催化材料。本文通过溶剂热法成功合成了一种具有酸度调节基团的新型光催化剂HSO-MIL-53(Fe)，并将其应用于去除卡马西平（CBZ）和布洛芬（IBP）。当pH值为8或9时，vis/HO/HSO-MIL-53(Fe)的光降解效率可达100%。自由基捕获实验和电子顺磁共振分析证明，空穴（h）、羟基自由基（·OH）、单线态氧（O）和超氧自由基（·O）是污染物降解的主要活性物种。在vis/HO/HSO-MIL-53(Fe)体系中，碱性条件下较高的污染物降解效率归因于两个因素：（1）酸度调节基团-HSO调节了整个体系的pH值，有利于光芬顿过程。（2）HSO-MIL-53(Fe)的光生电子可被Fe（III）、HO和O捕获，加速Fe（III）的还原并生成·OH、O和·O。此外，HO也可被Fe（II）和Fe（III）活化。上述过程协同提高了光催化效率。基于液相色谱-质谱（LC-MS）分析，提出了两种污染物可能的降解途径。
