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氧化铈纳米颗粒和氧化石墨烯掺杂聚丙烯酰胺对水溶液中亚甲基蓝染料的高效光催化降解

Efficient Photocatalytic Degradation of Methylene Blue Dye from Aqueous Solution with Cerium Oxide Nanoparticles and Graphene Oxide-Doped Polyacrylamide.

作者信息

Kalaycıoğlu Zeynep, Özuğur Uysal Bengü, Pekcan Önder, Erim F Bedia

机构信息

Department of Chemistry, Faculty of Science and Letters, Istanbul Technical University, Maslak, Istanbul 34469, Turkey.

Faculty of Engineering and Natural Sciences, Kadir Has University, Cibali, Fatih, Istanbul 34083, Turkey.

出版信息

ACS Omega. 2023 Mar 29;8(14):13004-13015. doi: 10.1021/acsomega.3c00198. eCollection 2023 Apr 11.

Abstract

A cerium oxide nanoparticles (CeO-NPs)/graphene oxide (GO)/polyacrylamide (PAM) ternary composite was synthesized through free-radical polymerization of acrylamide in the presence of CeO nanoparticles and GO in an aqueous system. The synthesized composite material was characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, scanning electron microscopy (SEM), and energy-dispersive X-ray (EDX) spectroscopy techniques and applied for the photocatalytic degradation of methylene blue (MB) dye from an aqueous solution. Tauc's model for direct transition was used to model for the optical band gap. The key operating parameters such as the amounts of CeO-NPs and GO, pH, initial MB concentration, type of light irradiation, and contact time have been optimized to achieve the highest MB degradation percentage. The photocatalysis process was pH-dependent, and the optimum pH value was found to be 12.0. Under UV-A light, 90% dye degradation occurred in 90 min. The degradation of MB was also specified in terms of total organic carbon (TOC) and chemical oxygen demand (COD). Free-radical capture experiments were also performed to determine the role of radical species during the photocatalytic oxidation process. The photocatalytic process showed that the equilibrium data is in good agreement with the Langmuir-Hinshelwood kinetic model. A rate constant of 0.0259 min was obtained. The hydrogel was also tested to assess its reusability, which is an important key factor in practical wastewater treatment. The photocatalytic activity only decreased to 75% after nine uses.

摘要

通过在水体系中,在氧化铈纳米颗粒(CeO-NPs)和氧化石墨烯(GO)存在下丙烯酰胺的自由基聚合反应,合成了一种氧化铈纳米颗粒/氧化石墨烯(GO)/聚丙烯酰胺(PAM)三元复合材料。通过X射线衍射(XRD)、傅里叶变换红外(FTIR)光谱、扫描电子显微镜(SEM)和能量色散X射线(EDX)光谱技术对合成的复合材料进行了表征,并将其应用于水溶液中亚甲基蓝(MB)染料的光催化降解。采用Tauc直接跃迁模型对光学带隙进行建模。对CeO-NPs和GO的用量、pH值、初始MB浓度、光照类型和接触时间等关键操作参数进行了优化,以实现最高的MB降解率。光催化过程依赖于pH值,发现最佳pH值为12.0。在UV-A光下,90分钟内染料降解率达到90%。还从总有机碳(TOC)和化学需氧量(COD)方面对MB的降解进行了说明。还进行了自由基捕获实验,以确定光催化氧化过程中自由基物种的作用。光催化过程表明,平衡数据与Langmuir-Hinshelwood动力学模型吻合良好。获得的速率常数为0.0259 min⁻¹。还对水凝胶的可重复使用性进行了测试,这是实际废水处理中的一个重要关键因素。经过九次使用后,光催化活性仅降至75%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c2d7/10099124/ef6f135a7ac6/ao3c00198_0002.jpg

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