Optimized Cu2O-{100} facet for generation of different reactive oxidative species via peroxymonosulfate activation at specific pH values to efficient acetaminophen removal

IF 6.1 3区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nanotechnology Reviews Pub Date : 2023-01-01 DOI:10.1515/ntrev-2022-0542

Ke Chen, Xudong Yang, Rui Hao, Minghui Shao, Xiaoyong Yang, Xiuze Li, Yuxuan Li, Juzhe Liu, Sai Zhang

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Abstract

Abstract Activation of peroxymonosulfate (PMS) to degrade persistent organic contaminants has received increasing attention in wastewater purification. In this study, Cu2O catalysts with different exposed crystal facets were prepared, characterized, and evaluated for acetaminophen (ACE) degradation through PMS activation. The experimental results showed that cubic Cu2O with {100} facets exhibited remarkable activity on ACE removal by PMS activation in wide pH range of 3–11. DFT calculations indicated that Cu2O-{100} displayed higher electron transfer efficiency and PMS adsorption ability, further improving PMS activation. The radicals quenching experiments and electron paramagnetic resonance (EPR) results illustrated that singlet oxygen (1O2) was dominant reactive oxidative species (ROSs) during oxidation reactions and the relevant generation pathways were distinctly elucidated. Finally, the possible PMS activation mechanisms were discussed for ACE degradation in a wide pH range. This study will provide new insights to disclose PMS-based advanced oxidation processes (AOPs), and offer a new approach for wastewater purification by non-radical reactions.

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优化Cu2O-{100}面，通过在特定pH值下活化过氧一硫酸盐产生不同的反应性氧化物种，以有效去除对乙酰氨基酚

摘要过氧一硫酸盐（PMS）的活化降解持久性有机污染物在废水净化中受到越来越多的关注。在本研究中，制备了具有不同暴露晶面的Cu2O催化剂，对其进行了表征，并通过PMS活化对乙酰氨基酚（ACE）的降解进行了评估。实验结果表明，在3–11的宽pH范围内，具有{100}晶面的立方Cu2O对PMS活化去除ACE表现出显著的活性。DFT计算表明，Cu2O-{100}表现出更高的电子转移效率和PMS吸附能力，进一步提高了PMS的活性。自由基猝灭实验和电子顺磁共振（EPR）结果表明，在氧化反应中，单线态氧（1O2）是主要的反应性氧化物种（ROS），并清楚地阐明了相关的生成途径。最后，讨论了PMS在宽pH范围内降解ACE的可能激活机制。这项研究将为揭示基于PMS的高级氧化工艺（AOPs）提供新的见解，并为通过非自由基反应净化废水提供一种新的方法。

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来源期刊

Nanotechnology Reviews CHEMISTRY, MULTIDISCIPLINARY-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

11.40

自引率

13.50%

发文量

137

审稿时长

7 weeks

期刊介绍： The bimonthly journal Nanotechnology Reviews provides a platform for scientists and engineers of all involved disciplines to exchange important recent research on fundamental as well as applied aspects. While expert reviews provide a state of the art assessment on a specific topic, research highlight contributions present most recent and novel findings. In addition to technical contributions, Nanotechnology Reviews publishes articles on implications of nanotechnology for society, environment, education, intellectual property, industry, and politics.