Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, China.
Int J Mol Sci. 2023 May 27;24(11):9378. doi: 10.3390/ijms24119378.
In this work, the MnFeO/BGA (boron-doped graphene aerogel) composite prepared via the solvothermal method is applied as a photocatalyst to the degradation of tetracycline in the presence of peroxymonosulfate. The composite's phase composition, morphology, valence state of elements, defect and pore structure were analyzed by XRD, SEM/TEM, XPS, Raman scattering and N adsorption-desorption isotherms, respectively. Under the radiation of visible light, the experimental parameters, including the ratio of BGA to MnFeO, the dosages of MnFeO/BGA and PMS, and the initial pH and tetracycline concentration were optimized in line with the degradation of tetracycline. Under the optimized conditions, the degradation rate of tetracycline reached 92.15% within 60 min, whereas the degradation rate constant on MnFeO/BGA remained 4.1 × 10 min, which was 1.93 and 1.56 times of those on BGA and MnFeO, respectively. The largely enhanced photocatalytic activity of the MnFeO/BGA composite over MnFeO and BGA could be ascribed to the formation of type I heterojunction on the interfaces of BGA and MnFeO, which leads to the efficient transfer and separation of photogenerated charge carriers. Transient photocurrent response and electrochemical impedance spectroscopy tests offered solid support to this assumption. In line with the active species trapping experiments, SO and O radicals are confirmed to play crucial roles in the rapid and efficient degradation of tetracycline, and accordingly, a photodegradation mechanism for the degradation of tetracycline on MnFeO/BGA is proposed.
在这项工作中,通过溶剂热法制备的 MnFeO/BGA(掺硼石墨烯气凝胶)复合材料被用作光催化剂,在过一硫酸盐存在下用于降解四环素。通过 XRD、SEM/TEM、XPS、拉曼散射和 N 吸附-脱附等温线分别分析了复合材料的物相组成、形貌、元素价态、缺陷和孔结构。在可见光辐射下,实验参数,包括 BGA 与 MnFeO 的比例、MnFeO/BGA 和 PMS 的用量以及初始 pH 值和四环素浓度,均根据四环素的降解进行了优化。在优化条件下,四环素在 60 分钟内的降解率达到 92.15%,而 MnFeO/BGA 上的降解速率常数保持在 4.1×10-2 min-1,分别是 BGA 和 MnFeO 的 1.93 和 1.56 倍。MnFeO/BGA 复合材料相对于 MnFeO 和 BGA 具有较大增强的光催化活性,可归因于 BGA 和 MnFeO 界面上形成的 I 型异质结,这导致光生载流子的有效转移和分离。瞬态光电流响应和电化学阻抗谱测试为此假设提供了有力支持。根据活性物质捕获实验,SO 和 O 自由基被确认为在四环素的快速和有效降解中起关键作用,因此,提出了 MnFeO/BGA 上降解四环素的光降解机理。