Two-dimensional ultrathin perforated Co3O4 nanosheets enhanced PMS-Activated selective oxidation of organic micropollutants in environmental remediation

催化作用 双酚A 纳米片 化学 四溴双酚A 腐植酸 降级(电信) 激进的 猝灭(荧光) 多孔性 电子顺磁共振 化学工程 光化学 无机化学 有机化学 荧光 计算机科学 肥料 核磁共振 量子力学 阻燃剂 环氧树脂 电信 工程类 物理
作者
Qiao Wang,Zetao Xu,Yiting Cao,Yuanqing Chen,Xing Du,Yang Yang,Zhihong Wang
出处
期刊:Chemical Engineering Journal [Elsevier]
卷期号:427: 131953-131953 被引量:71
标识
DOI:10.1016/j.cej.2021.131953
摘要

Here a two-dimensional (2D) ultrathin perforated Co3O4 nanosheet is rationally designed by a wet-chemical synthesis to activate peroxymonosulfate (PMS) for efficient selective oxidation. And the physicochemical properties of catalyst were investigated by series of techniques. The Co3O4 nanosheets achieved a 98.0% degradation efficiency of bisphenol A (BPA) within 30 min, showing a 4 times higher kinetic constant (0.112 min−1) and 5 times lower Co2+ leakage (6.5 μg/L), than commercial Co3O4 microspheres. The great enhancement in catalytic performance was ascribed to the large surface area and pore diameter in porous 2D structure, as well as the strong electrostatic attraction with PMS. Moreover, the influence of several parameters such as initial pH, temperatures, humic acids and inorganic anions in the system on the remaval of BPA were systematically studied. Since sulfate radicals (SO4−) were proved to be the primary reactive oxygen species by EPR measurements and quenching experiments, the PMS/Co3O4 nanosheets exhibits a highly selective oxidation on aromatics with electron donating groups (i.e., –OH and –CH3), while a relatively low value for organics with electron-withdrawing groups (e.g., –NO2 and –COOH). A high ionization potential threshold was determined to be greater than 9.39 eV, corresponding to a high oxidation ability to react with the organics. Finally, possible degradation pathways were proposed based on twenty intermediate products determined from mass spectrometry.
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