锰
化学
催化作用
激进的
氧气
单线态氧
反应速率常数
氧化还原
矿化(土壤科学)
降级(电信)
猝灭(荧光)
吸附
光化学
无机化学
有机化学
动力学
氮气
荧光
电信
物理
量子力学
计算机科学
作者
Weibao Liu,Ying Yang,Yunhe Li,Yuerong Zhou,Ce Wang,Yingtang Zhou,Jiangwei Shang,Xiuwen Cheng
标识
DOI:10.1016/j.seppur.2023.125015
摘要
The preparation of sulfate-based advanced oxidation catalysts is usually both complex and expensive. In this study, natural manganese sand enriched with oxygen vacancies was prepared by NaBH4 reduction of natural manganese sand for activating peroxymonosulfate (PMS) to remove carbamazepine (CBZ). 70% of carbamazepine was degraded at 120 min when natural manganese sand enriched with oxygen vacancies and PMS were dosed at 0.4 g/L and 0.3 g/L respectively, and the reaction rate constant of the natural manganese sand system with rich oxygen vacancies was 7 times that of the common system. The mineralization of total organic carbon (TOC) reached 41.9%. Combined EPR and radical quenching assays revealed that degradation of pollutants relied on the involvement of free radicals and non-free radicals, in which singlet oxygen was dominant. The XPS results showed that the redox cycles of Fe3+/Fe2+ and Mn4+/Mn3+/Mn2+ promoted the generation of free radicals. Density functional theory results also showed that the energy required for PMS to adsorb on natural manganese sand with many oxygen vacancies was decreased, and the OO bond was elongated, which was beneficial to the catalytic reaction. According to LC-MS and Fukui function, the degradation route of CBZ was predicted, and the toxicity of the breakdown products was calculated. The research provides a reference for introducing oxygen vacancies in natural catalysts to improve degradation performance for "green (source) to green (application)".
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