School of Materials Science and Engineering, Beihang University, Beijing, 100191, PR China; State Key Laboratory of Advanced Metallurgy, School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083, PR China.
State Key Laboratory of Advanced Metallurgy, School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083, PR China.
J Environ Manage. 2022 Nov 1;321:115907. doi: 10.1016/j.jenvman.2022.115907. Epub 2022 Aug 20.
A novel metal doped MgFeO@g-CN (m-MF@CN) nanocomposite was synthesized by one-pot method using saprolite laterite nickel ore and urea as raw materials. The heterostructure was verified as an effective heterogeneous Fenton-like catalyst for degrading antibiotics including tetracycline, oxytetracycline and chlortetracycline hydrochloride, and the related catalytic mechanism was elaborated in detail. Under the optimum conditions, the m-MF@CN/HO/vis system exhibited superior photo-Fenton property (degradation efficiency of 93.15% within 30 min, TOC removal efficiency was as high as 60.54% within 120 min) and cycle stability for tetracycline removal. The combination of MgFeO and g-CN enhanced the absorption of visible light, and the energy level matched heterojunction promoted the separation of photogenerated electron-holes to accelerate the redox cycle of ≡Fe/≡Fe. Free radical quenching and electron spin resonance (ESR) analysis confirmed that O was the main active species, h and OH also played a synergistic role in the degrading reactions. Notably, a possible degradation pathway of tetracycline was proposed according to the intermediates produced in the reaction process. The one-step synthesized m-MF@CN nanocomposite catalysts possessed high catalytic performance, good stability and recoverability, which not only realized the high-value utilization of ore raw materials, but also provided a potential practical way for efficient treatment of antibiotic wastewater.
采用共沉淀法以钛铁矿和尿素为原料合成了一种新型的金属掺杂 MgFeO@g-CN(m-MF@CN)纳米复合材料。该复合材料被证实为一种有效的非均相类 Fenton 催化剂,可用于降解四环素、土霉素和盐酸金霉素等抗生素,详细阐述了相关的催化机制。在最佳条件下,m-MF@CN/HO/vis 体系对四环素的去除具有优越的光 Fenton 性能(30 分钟内降解效率达到 93.15%,120 分钟内TOC 去除效率高达 60.54%)和循环稳定性。MgFeO 和 g-CN 的结合增强了可见光的吸收,能级匹配的异质结促进了光生电子-空穴的分离,从而加速了≡Fe/≡Fe 的氧化还原循环。自由基淬灭和电子自旋共振(ESR)分析证实,O 是主要的活性物质,h 和 OH 也在降解反应中发挥协同作用。根据反应过程中产生的中间体,提出了一种可能的四环素降解途径。一步法合成的 m-MF@CN 纳米复合材料催化剂具有高催化性能、良好的稳定性和可回收性,不仅实现了矿石原料的高价值利用,而且为高效处理抗生素废水提供了一种潜在的实用方法。