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一种新颖的 Sm 掺杂 CrO3 修饰的 MWCNTs 异质结构 Fenton 样催化剂,在可见光照射下具有声光电芬顿催化活性。

A novel Sm doped CrO sesquioxide-decorated MWCNTs heterostructured Fenton-like with sonophotocatalytic activities under visible light irradiation.

机构信息

Department of Separation Science, School of Engineering Science, Lappeenranta University of Technology, Sammonkatu 12, FI-50130 Mikkeli, Finland; Petrochemicals department, Egyptian Petroleum Research Institute, Nasr City, Cairo 11727, Egypt.

Division of Cardiac Surgery, Heart Centre Siegburg-Wuppertal, University Witten, Herdecke, Germany.

出版信息

J Hazard Mater. 2022 Mar 15;426:127812. doi: 10.1016/j.jhazmat.2021.127812. Epub 2021 Nov 21.

Abstract

Novel Sm doped CrO decorated MWCNTs nanocomposite photocatalyst was successfully prepared by a facile hydrothermal method for metoprolol (MET) degradation. A heterogeneous photo -Fenton like system was formed with the addition of HO for ultrasonic irradiation (US), visible light irradiation (Vis) and dual irradiation (US/Vis) systems. The intrinsic characteristics of Sm doped CrO decorated MWCNTs nanocomposite was comprehensively performed using state-of-art characterization tools. Optical studies confirmed that Sm doping shifted the absorbance of CrO towards the visible-light region, further enhanced by MWCNTs incorporation. In this study, degradation of metoprolol (MET) was investigated in the presence of CrO nanoparticles, Sm doped CrO and Sm doped CrO decorated MWCNTs nanocomposites using sonocatalysis and photocatalysis and simultaneously. Several different experimental parameters, including irradiation time, HO concentration, catalyst amount, initial concentration, and pH value, were optimized. The remarkably enhanced sonophotocatalytic activity of Sm doped CrO decorated MWCNTs could be attributed to the more formation of reactive radicals and the excellent electronical property of Sm doping and MWCNTs. The rate constant of degradation using sonophotocatalytic system was even higher than the sum of rates of individual systems due to its synergistic performance based on the kinetic data. A plausible mechanism for the degradation of MET over Sm-CrO/MWCNTs is also demonstrated by using active species scavenger studies and EPR spectroscopy. Our findings imply that (OH), (h) and (O) were the reactive species responsible for the degradation of MET based on the special three-way Fenton-like mechanism and the dissociation of HO. The durability and stability of the nanocomposite were also performed, and the obtained results revealed that the catalysts can endure the harsh sonophotocatalytic conditions even after fifth cycles. Mineralization experiments using the optimized parameters were evaluated as well. The kinetics and the reaction mechanism with the possible reasons for the synergistic effect were presented. Identification of degraded intermediates also investigated.

摘要

新型 Sm 掺杂 CrO 修饰 MWCNTs 纳米复合材料光催化剂通过简便的水热法成功制备,用于美托洛尔 (MET) 的降解。通过添加 HO 形成了非均相光芬顿类似体系,用于超声辐照 (US)、可见光辐照 (Vis) 和双辐照 (US/Vis) 体系。使用最先进的表征工具对 Sm 掺杂 CrO 修饰 MWCNTs 纳米复合材料的固有特性进行了全面研究。光学研究证实,Sm 掺杂将 CrO 的吸光度向可见光区域移动,进一步通过 MWCNTs 的掺入增强。在这项研究中,在 CrO 纳米颗粒、Sm 掺杂 CrO 和 Sm 掺杂 CrO 修饰 MWCNTs 纳米复合材料的存在下,通过声催化和光催化同时研究了美托洛尔 (MET) 的降解。优化了几种不同的实验参数,包括辐照时间、HO 浓度、催化剂用量、初始浓度和 pH 值。Sm 掺杂 CrO 修饰 MWCNTs 的显著增强的声光电催化活性可归因于更多的活性自由基的形成和 Sm 掺杂和 MWCNTs 的优异电子性能。根据动力学数据,基于协同性能,声光电催化系统的降解速率常数甚至高于各个系统的速率之和。通过使用活性物质清除剂研究和 EPR 光谱,也证明了 MET 在 Sm-CrO/MWCNTs 上降解的可能机制。我们的研究结果表明,基于特殊的三向芬顿类似机制和 HO 的解离,(OH)、(h) 和 (O) 是 MET 降解的活性物质。还进行了纳米复合材料的耐用性和稳定性研究,所得结果表明,即使经过五次循环,催化剂也能承受苛刻的声光电催化条件。还评估了使用优化参数的矿化实验。提出了动力学和反应机制以及协同效应的可能原因。还研究了降解中间体的鉴定。

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