Catalytic activation of peroxodisulfate using shape-controlled cerium-manganese composite oxide for phenol degradation: Kinetics and degradation pathway investigation

IF 7.2 1区化学 Q1 CHEMISTRY, APPLIED Journal of Rare Earths Pub Date : 2024-08-01 Epub Date: 2023-10-20 DOI:10.1016/j.jre.2023.10.008

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Abstract

Phenol-containing wastewater is typical organic wastewater, and its treatment is arduous. An advanced method to treat this type of wastewater is persulfate activation. Environmentally friendly cerium-manganese composite oxide materials were synthesized by hydrothermal method and applied to the phenol degradation process. Various ratios of cerium and manganese, as well as the amount of sodium hydroxide, were investigated. The solid solutions of cerium and manganese were formed and confirmed by X-ray diffraction (XRD) and transmission electron microscopy (TEM). H₂-temperature programmed reduction (H₂-TPR) and X-ray photoelectron spectroscopy (XPS) were utilized to analyze the synergistic effect of cerium and manganese. It is found that there is a transformation between Ce⁴⁺/Ce³⁺ and Mn²⁺/Mn³⁺, which makes the material more trivalent manganese and thereby increases the catalytic activity. The effect of materials in catalyzing phenol degradation by peroxodisulfate (PDS) under various preparation conditions is discussed and high-efficiency removal of phenol can be achieved and the removal rate at 180 min is close to 100%. The kinetic of this process was investigated and activation energy of phenol degradation is 62.35 kJ/mol. The degradation pathway of phenol was studied and it is found that PDS can be activated by low metal ions and the ·OH and SO₄·^– radicals play crucial roles according to the quenching experiments.

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利用形状可控的铈锰复合氧化物催化活化过二硫酸盐以降解苯酚：动力学和降解途径研究

含酚废水是典型的有机废水，其处理过程十分复杂。处理这类废水的先进方法是过硫酸盐活化法。本研究采用水热法合成了环保型铈锰复合氧化物材料，并将其应用于苯酚降解过程。研究了不同比例的铈和锰以及氢氧化钠的用量。铈和锰形成了固溶体，并通过 X 射线衍射 (XRD) 和透射电子显微镜 (TEM) 得到了证实。利用 H2 温度编程还原（H2-TPR）和 X 射线光电子能谱（XPS）分析了铈和锰的协同效应。研究发现，Ce4+/Ce3+ 和 Mn2+/Mn3+ 之间存在转化，这使得材料中的三价锰含量增加，从而提高了催化活性。讨论了材料在不同制备条件下催化过二硫酸盐（PDS）降解苯酚的效果，结果表明可以高效去除苯酚，180 分钟的去除率接近 100%。对这一过程的动力学进行了研究，苯酚降解的活化能为 62.35 kJ/mol。对苯酚的降解途径进行了研究，发现 PDS 可被低金属离子激活，根据淬灭实验，-OH 和 SO4--自由基起着关键作用。

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文献相关原料

公司名称

产品信息

阿拉丁

cerium nitrate hexahydrate

阿拉丁

sodium hydroxide

阿拉丁

phenol

来源期刊

Journal of Rare Earths 化学-应用化学

CiteScore

8.70

自引率

14.30%

发文量

374

审稿时长

1.7 months

期刊介绍： The Journal of Rare Earths reports studies on the 17 rare earth elements. It is a unique English-language learned journal that publishes works on various aspects of basic theory and applied science in the field of rare earths (RE). The journal accepts original high-quality original research papers and review articles with inventive content, and complete experimental data. It represents high academic standards and new progress in the RE field. Due to the advantage of abundant RE resources of China, the research on RE develops very actively, and papers on the latest progress in this field emerge every year. It is not only an important resource in which technicians publish and obtain their latest research results on RE, but also an important way of reflecting the updated progress in RE research field. The Journal of Rare Earths covers all research and application of RE rare earths including spectroscopy, luminescence and phosphors, rare earth catalysis, magnetism and magnetic materials, advanced rare earth materials, RE chemistry & hydrometallurgy, RE metallography & pyrometallurgy, RE new materials, RE solid state physics & solid state chemistry, rare earth applications, RE analysis & test, RE geology & ore dressing, etc.