Green synthesis of magnetic type Zeolites 4A as catalyst for the elimination of quinoline yellow by the Fenton process: Optimization and kinetic investigation

Hybrid Advances Pub Date : 2025-06-01 Epub Date: 2025-02-05 DOI:10.1016/j.hybadv.2025.100401
Roland Urselin Noumsi Foko , Cyrille Ghislain Fotsop , Donald Raoul Tchuifon Tchuifon , Charles Banenzoué , Anatole Guy Blaise Azebaze
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Abstract

This work describes the hydrothermal synthesis and characterization of zeolite 4A (Zeo-4A) and magnetite zeolite (Zeo-4A@Fe3O4) from Cameroonian raw kaolin. The study also explores the efficiency of Zeo-4A@Fe3O4 for the removal of quinoline yellow (E104) via Fenton process. XRD, FTIR, SEM, EDX, NMR-MAS and TGA-DSC characterizations show that Zeo-4A is crystalline with cubic morphology, while Zeo-4A@Fe3O4 exhibits a bonding interaction between zeolite and Fe3O4 nanoparticle leading to morphological structural changes. The degradation of quinoline yellow by heterogeneous Fenton process was carried out by varying several parameters, namely solution pH (3–7), H2O2 concentration (0.5–1.5 mol/L), quinoline yellow concentration (50–100 mg/L), and catalyst mass (50–100 mg). The results of catalytic performance tests reveal that the degradation efficiency of synthetic Zeo-4A, Zeo-4A@Fe3O4 and Fe3O4 were 1.71 %, 93.60 % and 92.65 %, respectively, after 60 min. Confirmatory tests were carried out by response surface methodology based on the Box-Behnken design, and a degradation rate of 98.81 % was obtained under optimum conditions of pH 3.84, 50.14 mg/L, 100 mg, and 1.5 g/L; which is well in line with the model predictions. A significant quadratic regression model R2 = 91.35 % and the adjusted coefficient of determination value (adjusted R2 = 82.04 %) were observed using the analysis of the variance. The study of catalyst recovery and reusability shows that the catalysts remain stable with a degradation rate greater than 66 % after five cycles. The kinetics results show that the degradation of E104 follows first and second order kinetic models, influenced by pH and catalyst mass, with optimum efficiency at pH 3. The characterization results of the material after degradation show that it maintains its structural integrity after use.
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Fenton法绿色合成磁性4A型沸石消除喹啉黄的优化及动力学研究
本文描述了用喀麦隆原料高岭土水热合成4A沸石(Zeo-4A)和磁铁矿沸石(Zeo-4A@Fe3O4)并对其进行表征。研究还探讨了Zeo-4A@Fe3O4 Fenton法去除喹啉黄(E104)的效率。XRD、FTIR、SEM、EDX、NMR-MAS和TGA-DSC表征表明,Zeo-4A为立方晶型,而Zeo-4A@Fe3O4表现出沸石与Fe3O4纳米颗粒之间的键合作用,导致形貌结构发生变化。通过改变溶液pH(3 ~ 7)、H2O2浓度(0.5 ~ 1.5 mol/L)、喹啉黄浓度(50 ~ 100 mg/L)、催化剂质量(50 ~ 100 mg)等参数,对非均相Fenton法降解喹啉黄进行了研究。催化性能测试结果表明,合成的Zeo-4A、Zeo-4A@Fe3O4和Fe3O4在60 min后的降解效率分别为1.71%、93.60%和92.65%。基于Box-Behnken设计的响应面法进行了验证试验,在pH为3.84、50.14 mg/L、100 mg和1.5 g/L的最佳条件下,降解率为98.81%;这与模型预测非常吻合。方差分析得到显著的二次回归模型R2 = 91.35%,调整后的决定值系数R2 = 82.04%。催化剂的回收和重复使用研究表明,经过5次循环后,催化剂保持稳定,降解率大于66%。动力学结果表明,E104的降解符合一阶和二阶动力学模型,受pH和催化剂质量的影响,pH为3时效果最佳。降解后的表征结果表明,该材料在使用后仍保持其结构完整性。
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