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负载 Fe-Cu 二元氧化物的沸石作为非均相 Fenton 催化剂,在近中性 pH 条件下降解卡马西平。

Fe-Cu binary oxide loaded zeolite as heterogeneous Fenton catalyst for degradation of carbamazepine at near-neutral pH.

机构信息

Department of Environmental Science and Engineering, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.

出版信息

Environ Sci Pollut Res Int. 2022 Oct;29(48):73181-73190. doi: 10.1007/s11356-022-20299-7. Epub 2022 May 27.

Abstract

In this study, Fe-Cu binary oxide was loaded on zeolite (Fe/Cu/zeolite) to be used as heterogeneous Fenton catalyst, and the catalytic degradation of carbamazepine (CBZ) were optimized at near-neutral pH. The results showed that the Fe and Cu oxide, mainly FeO, FeO, and CuO nanoparticles, were uniformly distributed on the surface of zeolite particles. Under the optimized conditions, Fe/Cu/zeolite could completely degrade CBZ when initial pH ranged from 3 to 7, and the removal efficiency of CBZ still remained above 74% even though the initial pH increased to near 10. After 8 times' repeated use, the Fe/Cu/zeolite exhibited an over 95% removal efficiency of CBZ. The hydroxyl radicals (•OH) were verified to be the main active oxidants by quenching experiments and ESR testing. The XPS of the materials revealed that the high catalytic efficiency was attributed to the synergistic effect of Fe(III)/Fe(II) and Cu(II)/Cu(I) redox cycles. This catalyst can be used for the efficient degradation of organic pollutants in heterogeneous Fenton systems.

摘要

在这项研究中,将 Fe-Cu 二元氧化物负载在沸石上(Fe/Cu/zeolite),用作非均相芬顿催化剂,并在近中性 pH 下优化了卡马西平(CBZ)的催化降解。结果表明,Fe 和 Cu 氧化物,主要是 FeO、FeO 和 CuO 纳米颗粒,均匀分布在沸石颗粒表面。在优化条件下,Fe/Cu/zeolite 可在初始 pH 值为 3 至 7 范围内完全降解 CBZ,并且即使初始 pH 值增加到近 10,CBZ 的去除效率仍保持在 74%以上。重复使用 8 次后,Fe/Cu/zeolite 对 CBZ 的去除效率仍超过 95%。通过猝灭实验和 ESR 测试验证了羟基自由基(•OH)是主要的活性氧化剂。材料的 XPS 表明,高催化效率归因于 Fe(III)/Fe(II)和 Cu(II)/Cu(I)氧化还原循环的协同作用。该催化剂可用于非均相芬顿体系中有效降解有机污染物。

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