High-efficiency Cu2O/CuFe-LDH nanocomposite for Fenton degradation of organic pollutants: Boosted dual redox cycles

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL
Yanrui Su , Xiaoyu Li , Zimu Gao , Jiajia He , Zizhen Liu , Linjun Duan , Tian Sun , Jiaoge Wu , Dan Liang , Chaojun Wei , Faying Fan , Wa Gao
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Abstract

The incorporation of dual redox sites within catalytic materials for H2O2 activation represents a promising approach to enhance the efficiency of pollutant decomposition. In this study, Cu2O modified CuFe-LDH nanocomposite (Cu2O/CuFe-LDH) was successfully synthesized via in situ topotactic transformation of CuFe-LDH. The catalytic degradation performance of the Cu2O/CuFe-LDH nanocomposite was investigated utilizing tetracycline hydrochloride (TCH) as a typical antibiotic contaminant. It demonstrated exceptional catalytic activity, achieving a TCH elimination rate of 93.0 % in 60 min. A rate constant value of 0.0426 min−1 was calculated for the pseudo-first-order kinetic model, which was 1.6 times and 5.0 times higher than those of CuFe-LDH and Cu2O, respectively. Moreover, the Cu2O/CuFe-LDH nanocomposite demonstrated remarkable cycling stability (85 % degradation rate after 5 recycling cycles), a wide pH range (3−11), resistance to background ion interference, and lower toxicity of the products of degradation. Based on radical scavenger tests and electron paramagnetic resonance (EPR) spectroscopy, it was verified that TCH degradation was mediated by 1O2, •OH and •O2-, with 1O2 playing an essential role. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) investigations indicate that the remarkable catalytic efficacy of Cu2O/CuFe-LDH is predominantly due to the synergistic interactions between Cu2O and CuFe-LDH, with Cu2O promoting the accelerated dual Cu2+/Cu+ and Fe3+/Fe2+ cycling. Thus, the Cu2O/CuFe-LDH nanocomposite exhibits exceptional efficiency, environmental friendliness and recyclability, rendering it an ideal candidate for practical wastewater treatment applications.
高效Cu2O/CuFe-LDH纳米复合材料Fenton降解有机污染物:促进双氧化还原循环
在催化材料中加入双氧化还原位点进行H2O2活化是提高污染物分解效率的一种很有前途的方法。在本研究中,通过CuFe-LDH的原位拓扑转化,成功合成了Cu2O修饰CuFe-LDH纳米复合材料(Cu2O/CuFe-LDH)。以盐酸四环素为典型抗生素污染物,研究了Cu2O/CuFe-LDH纳米复合材料的催化降解性能。它表现出优异的催化活性,在60 min内达到93.0 %的TCH去除率。拟一级动力学模型的速率常数为0.0426 min−1,分别是CuFe-LDH和Cu2O的1.6倍和5.0倍。此外,Cu2O/CuFe-LDH纳米复合材料具有显著的循环稳定性(5次循环后降解率为85% %),pH范围宽(3 ~ 11),耐本底离子干扰,降解产物毒性低。通过自由基清除试验和电子顺磁共振(EPR)谱分析,证实了TCH的降解是由1O2、•OH和•O2-介导的,其中1O2起重要作用。x射线光电子能谱(XPS)和密度泛函理论(DFT)研究表明,Cu2O/CuFe-LDH的显著催化效果主要是由于Cu2O与CuFe-LDH之间的协同作用,其中Cu2O促进了Cu2+/Cu+和Fe3+/Fe2+的加速双循环。因此,Cu2O/CuFe-LDH纳米复合材料表现出卓越的效率、环境友好性和可回收性,使其成为实际废水处理应用的理想候选者。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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