School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu, People's Republic of China.
Oil & Gas Field Applied Chemistry Key Laboratory of Sichuan Province, Chengdu, People's Republic of China.
Environ Technol. 2024 Sep;45(22):4656-4669. doi: 10.1080/09593330.2023.2283054. Epub 2023 Nov 15.
A novel type of oxide material, high entropy oxide (MnFeCoNiCu)O (MFO) composites with spinel structure were successfully synthesized by a simple solution combustion in this paper, and it was first applied to the degradation of antibiotic organic pollutants in water by photo-Fenton. SEM and BET characterization showed that the composite was porous and had a large specific surface area. XPS results showed that Fe, Mn, Cu, Co and Ni all participated in the redox reaction of the catalytic process. The redox pairs of Mn/Mn, Cu/Cu, Co/Co, Ni/Ni can accelerate the Fe/Fe redox cycling in MFO to activate HO and produce more reactive oxygen species. The catalytic performance of MFO composite was investigated using tetracycline hydrochloride (TC-HCl) as a model pollutant. The results displayed that the degradation rate of TC-HCl by MFO was 92.9% when the initial pH was 4, the dose of HO was 50 mM, and the irradiation time was 60 min. The high entropy oxide MFO composites could build up an internal electric field, which restrains electron-hole recombination, improves the transfer of photogenerated charge carriers and maximize photocatalytic property. In addition, the free radical capture experiment determined that the main active species of the degradation reaction were e, •O and •OH. The synergistic effect of the five components in the high entropy oxide strengthens lattice distortion and defects, increases oxygen vacancies, and thus has enhanced catalytic effect for TC-HCl degradation. This work shows that high entropy oxides have excellent catalytic performance for tetracycline organic pollutants, and it is speculated that high entropy oxides have good application prospects in the field of advanced oxidation technology for the degradation of organic pollutants.
一种新型的氧化物材料，具有尖晶石结构的高熵氧化物（MnFeCoNiCu）O（MFO）复合材料，通过本文中的简单溶液燃烧成功合成，并首次应用于水中抗生素有机污染物的光芬顿降解。SEM 和 BET 表征表明，该复合材料具有多孔结构和较大的比表面积。XPS 结果表明，Fe、Mn、Cu、Co 和 Ni 都参与了催化过程的氧化还原反应。Mn/Mn、Cu/Cu、Co/Co、Ni/Ni 的氧化还原对可以加速 MFO 中的 Fe/Fe 氧化还原循环，激活 HO 并产生更多的活性氧物质。使用盐酸四环素（TC-HCl）作为模型污染物研究了 MFO 复合材料的催化性能。结果表明，当初始 pH 值为 4、HO 剂量为 50mM 且照射时间为 60min 时，MFO 对 TC-HCl 的降解率为 92.9%。高熵氧化物 MFO 复合材料可以建立内部电场，抑制电子-空穴复合，提高光生载流子的转移效率，并最大限度地提高光催化性能。此外，自由基捕获实验确定降解反应的主要活性物质是 e、•O 和•OH。高熵氧化物中五种成分的协同作用增强了晶格畸变和缺陷，增加了氧空位，从而对 TC-HCl 的降解具有增强的催化作用。这项工作表明，高熵氧化物对四环素有机污染物具有优异的催化性能，并推测高熵氧化物在有机污染物高级氧化技术降解领域具有良好的应用前景。
