Synthesis oxygen vacancies enriched CuO hierarchical nanosheets for peroxymonosulfate activation toward P-nitrophenol degradation and mechanism

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Dongyan Wang, Min Wang, Zhenqi Xu, Ying Hu, Jiwen Zhong, Taizhuo Ma
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Abstract

In this work, hierarchical copper oxide (CuO) nanosheet with rich oxygen vacancies was prepared with a facile biotemplates derivatization method. Results show that the as-prepared optimum CuO-II exhibited excellent catalytic performance for peroxymonosulfate (PMS) activation mainly benefiting from large specific surface area and electron transfer efficiency, abundant Cu+ and oxygen vacancies in catalyst. Almost 100 % of P-nitrophenol (PNP) can be degrade within 10 min by CuO-II activating PMS process. The electron paramagnetic resonance (EPR) spectroscopy, reactive species quenching tests and density functional theory (DFT) calculation results revealed that Cu(III)-mediated electron transfer and sulfate radicals were identified as the dominantly responsible for PNP degradation. Meanwhile, CuO-II/PMS system can degrade PNP in a wide range of pH (pH 3 ∼ 10) and with inorganic anions and natural organic matter presence. In addition, CuO-II catalyst has good stability and reusability and performed well toward PNP degradation in the continuous operation. This work not only obtained a facile preparation strategy for obtaining CuO catalyst with excellent catalytic performance, but also gave a new idea for studying the mechanism of CuO activating PMS.

Abstract Image

合成富含氧空位的 CuO 分层纳米片,用于过一硫酸盐活化降解对硝基苯酚及其机理
本研究采用简便的生物模板衍生法制备了富含氧空位的分层氧化铜(CuO)纳米片。结果表明,所制备的最优 CuO-II 对过氧化单硫酸盐(PMS)的活化具有优异的催化性能,这主要得益于催化剂中较大的比表面积和电子传递效率、丰富的 Cu+ 和氧空位。在 CuO-II 活化 PMS 的过程中,对硝基苯酚(PNP)几乎可以在 10 分钟内 100% 降解。电子顺磁共振(EPR)光谱、活性物种淬灭试验和密度泛函理论(DFT)计算的结果表明,Cu(III)介导的电子转移和硫酸根自由基是 PNP 降解的主要原因。同时,CuO-II/PMS 体系可在较宽的 pH 值范围(pH 值 3 ∼ 10)内降解 PNP,并可在无机阴离子和天然有机物存在的情况下降解 PNP。此外,CuO-II 催化剂具有良好的稳定性和可重复使用性,在连续操作中降解 PNP 的性能良好。这项工作不仅为获得催化性能优异的 CuO 催化剂提供了简便的制备策略,而且为研究 CuO 活化 PMS 的机理提供了新的思路。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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