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共掺杂介孔 CeO 纳米棒作为非均相催化剂高效活化过一硫酸盐氧化苯酚。

Efficient activation of peroxymonosulfate by Co-doped mesoporous CeO nanorods as a heterogeneous catalyst for phenol oxidation.

机构信息

State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580, People's Republic of China.

School of Chemistry and Chemical Engineering, Qinghai Normal University, Xining, 810008, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2021 Jun;28(22):27852-27863. doi: 10.1007/s11356-021-12605-6. Epub 2021 Jan 30.

DOI:10.1007/s11356-021-12605-6
PMID:33517528
Abstract

Sulfate radical-based advanced oxidation processes have received considerable attentions in the remediation of organic pollutants due to their high oxidation ability. In this study, a novel CoO/CeO catalyst was fabricated and employed as a peroxymonosulfate (PMS) activator to generate SO for phenol degradation. The CoO/CeO catalyst exhibited a good catalytic performance at a wide pH range of 3.4 to 10.8, and 100% phenol (20 mg/L) was removed within 50-min reaction under optimal conditions with 0.2 g/L catalyst and 2.0 g/L PMS at room temperature. The transformation products and total organic carbon during the degradation process were also determined. The quenching experiments and electron paramagnetic resonance spectra revealed that sulfate radical (SO) rather than other species such as singlet oxygen (O) and hydroxyl radical (OH) was primarily responsible for phenol degradation in the CoO/CeO/PMS system, and a rational mechanism was proposed. Moreover, the recycling experiments as well as low cobalt leaching concentration manifested satisfactory reusability and stability. The effects of various inorganic anions and natural organic matter in real water matrix on phenol oxidation were further evaluated. We believe that the CoO/CeO composites have promising applications of PMS activation for the degradation of organic pollutants in wastewater treatment.

摘要

基于硫酸盐自由基的高级氧化工艺因其具有较高的氧化能力而在有机污染物的修复中受到了广泛关注。在这项研究中,制备了一种新型的 CoO/CeO 催化剂,并将其用作过一硫酸盐 (PMS) 的活化剂来产生 SO 以降解苯酚。CoO/CeO 催化剂在很宽的 pH 值范围(3.4 至 10.8)内表现出良好的催化性能,在室温下,在最佳条件下(催化剂用量为 0.2 g/L,PMS 用量为 2.0 g/L),100%的苯酚(20 mg/L)在 50 分钟内被去除。还确定了降解过程中的转化产物和总有机碳。淬灭实验和电子顺磁共振谱表明,在 CoO/CeO/PMS 体系中,主要负责苯酚降解的是硫酸盐自由基 (SO),而不是单线态氧 (O)和羟基自由基 (OH) 等其他物质,并提出了一种合理的机制。此外,通过循环实验和低钴浸出浓度表明该催化剂具有良好的可重复使用性和稳定性。还进一步评估了实际水基质中各种无机阴离子和天然有机物对苯酚氧化的影响。我们相信,CoO/CeO 复合材料在利用 PMS 活化处理废水有机污染物方面具有广阔的应用前景。

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