Faculty of Health Sciences, University of Macau, Macau SAR, 999078, China.
School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, Southern University of Science and Technology, Shenzhen, 518055, China.
Small. 2021 Oct;17(43):e2101393. doi: 10.1002/smll.202101393. Epub 2021 Jun 23.
Antibiotics discharge has been a critical issue as the abuse in clinical disease treatment and aquaculture industry. Advanced oxidation process (AOPs) is regarded as a promising approach to degrade organic pollutants from wastewater, however, the catalysts for AOPs always present low activities, and uncontrollable porosities, thus hindering their further wider applications. In this work, an aliovalent-substitution strategy is employed in metal-organic framework (MOF) precursors assembly, aiming to introduce Co(II/III) into Ce-O clusters which could modify the structure of the clusters, then change the crystallization, enlarge the surface area, and regulate the morphology. The introduction of Co(II/III) also enlarges the pore size for mass transfer and enriches the active sites for the production of sulfate radicals (SO ) in MOF-derived catalysts, leading to excellent performance in antibiotics removal. Significantly, the CeO •Co O nanoflowers could efficiently enhance the generation of sulfate radical SO and promote the norfloxacin removal efficiency to 99% within 20 min. The CeO •Co O nanoflowers also present remarkable universality toward various antibiotics and organic pollutants. The aliovalent-substitution strategy is anticipated to find wide use in the exploration of high-performance MOF-derived catalysts for various applications.
抗生素排放一直是一个关键问题,无论是在临床疾病治疗还是水产养殖行业中滥用抗生素的情况。高级氧化工艺(AOPs)被认为是一种很有前途的方法,可以降解废水中的有机污染物,但 AOPs 的催化剂通常存在活性低、孔隙不可控等问题,从而阻碍了它们的进一步广泛应用。在这项工作中,采用了一种不等价取代策略来组装金属有机骨架(MOF)前体,旨在将 Co(II/III) 引入 Ce-O 簇中,从而改变簇的结构,然后改变结晶度、扩大比表面积并调节形态。Co(II/III) 的引入还增大了传质的孔径并丰富了 MOF 衍生催化剂中产生硫酸根自由基(SO )的活性位点,从而在去除抗生素方面表现出优异的性能。值得注意的是,CeO·CoO 纳米花可以有效地增强硫酸根自由基 SO 的生成,并在 20 分钟内将诺氟沙星的去除效率提高到 99%。CeO·CoO 纳米花还表现出对各种抗生素和有机污染物的显著通用性。这种不等价取代策略有望在探索用于各种应用的高性能 MOF 衍生催化剂方面得到广泛应用。