Activation of peroxymonosulfate by Fe–Mn-modified MWCNTs for selective decontamination: Formation of high-valent metal-oxo species and superoxide anion radicals

被引:9
作者
Tian Y. [1 ,2 ]
Li Y. [1 ,2 ]
Ying G.-G. [1 ,2 ]
Feng Y. [1 ,2 ]
机构
[1] SCNU Environmental Research Institute, Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety & MOE Key Laboratory of Theoretical Chemistry of Environment, South China Normal University, Guangzhou
[2] School of Environment, South China Normal University, University Town, Guangzhou
基金
中国国家自然科学基金;
关键词
FeMn/CNTs; High-valent metal-oxo species; Peroxymonosulfate; Selective oxidation; Superoxide anion radicals;
D O I
10.1016/j.chemosphere.2023.139458
中图分类号
学科分类号
摘要
The extensive presence of organic micropollutants in complex water matrices requires the development of selective oxidation technologies. In this study, a novel selective oxidation process was developed via the conjunction of FeMn/CNTs with peroxymonosulfate and successfully used to remove micropollutants such as sulfamethoxazole (SMX) and bisphenol A from aqueous solutions. FeMn/CNTs were prepared using a facile co-precipitation method, characterized using a series of surface characterization techniques, and then tested for pollutant removal. The results showed that the FeMn/CNTs had much greater reactivity than CNTs, manganese oxide, and iron oxide. The pseudo-first-order rate constant with FeMn/CNTs was more than 2.9–5.7 times that of the other tested materials. The FeMn/CNTs had great reactivity in a wide range of pH values from 3.0 to 9.0, with the best reactivity found at pH values of 5.0 and 7.0. High-valent metal-oxo species such as Fe(IV)[dbnd]O and Mn(IV)[dbnd]O and superoxide anion radicals were determined to be the reactive species and were responsible for the oxidation of SMX. These reactive species were selective; therefore, the overall removal performance of SMX was not obviously influenced by high levels of water components including chloride ions, bicarbonates, and natural organic matters. The results from this study may promote the design and application of selective oxidation technologies for micropollutant abatement. © 2023 Elsevier Ltd
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共 56 条
[1]  
Ali S., Rehman S.A.U., Luan H.-Y., Farid M.U., Huang H., Challenges and opportunities in functional carbon nanotubes for membrane-based water treatment and desalination, Sci. Total Environ., 646, pp. 1126-1139, (2019)
[2]  
Ball D.L., Edwards J.O., The kinetics and mechanism of the decomposition of caro's acid. I, J. Am. Chem. Soc., 78, pp. 1125-1129, (1956)
[3]  
Bataineh H., Pestovsky O., Bakac A., pH-induced mechanistic changeover from hydroxyl radicals to iron(IV) in the Fenton reaction, Chem. Sci., 3, pp. 1594-1599, (2012)
[4]  
Bernofsky C., Bandara B.M.R., Hinojosa O., Electron spin resonance studies of the reaction of hypochlorite with 5,5-dimethyl-1-pyrroline-N-oxide, Free Radic. Biol. Med., 8, pp. 231-239, (1990)
[5]  
Buxton G.V., Greenstock C.L., Helman W.P., Ross A.B., Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (⋅OH/⋅O<sup>−</sup>) in aqueous solution, J. Phys. Chem. Ref. Data, 17, pp. 513-886, (1988)
[6]  
Cruz-Alcalde A., Sans C., Esplugas S., Priority pesticides abatement by advanced water technologies: the case of acetamiprid removal by ozonation, Sci. Total Environ., 599-600, pp. 1454-1461, (2017)
[7]  
Deborde M., Rabouan S., Mazellier P., Duguet J.-P., Legube B., Oxidation of bisphenol A by ozone in aqueous solution, Water Res., 42, pp. 4299-4308, (2008)
[8]  
Dong H., Li Y., Wang S., Liu W., Zhou G., Xie Y., Guan X., Both Fe(IV) and radicals are active oxidants in the Fe(II)/peroxydisulfate process, Environ. Sci. Technol. Lett., 7, pp. 219-224, (2020)
[9]  
Du X., Li C., Zhao L., Zhang J., Gao L., Sheng J., Yi Y., Chen J., Zeng G., Promotional removal of HCHO from simulated flue gas over Mn-Fe oxides modified activated coke, Appl. Catal. B Environ., 232, pp. 37-48, (2018)
[10]  
Duan P., Ma T., Yue Y., Li Y., Zhang X., Shang Y., Gao B., Zhang Q., Yue Q., Xu X., Fe/Mn nanoparticles encapsulated in nitrogen-doped carbon nanotubes as a peroxymonosulfate activator for acetamiprid degradation, Environ. Sci.: Nano, 6, pp. 1799-1811, (2019)