Comparative studies on Fenton-like reactions catalyzed by Fe<sub>3</sub>O<sub>4</sub> loaded inside and outside halloysite nanotubes for the removal of organic pollutants

doi:10.1007/s11706-024-0673-0

2024, Vol. 18

Issue (1) : 240673 https://doi.org/10.1007/s11706-024-0673-0

Comparative studies on Fenton-like reactions catalyzed by Fe₃O₄ loaded inside and outside halloysite nanotubes for the removal of organic pollutants

Yang Li, Jia-Qi Zhou, Huan-Yan Xu(

), Li-Min Dong, Mao-Chang Cao, Lian-Wei Shan, Li-Guo Jin, Xiu-Lan He, Shu-Yan Qi

Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials, School of Materials Science and Chemical Engineering, Harbin University of Science and Technology, Harbin 150040, China

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Abstract

In this work, Fe₃O₄ nanoparticles (NPs) loaded inside and outside halloysite nanotubes (HNTs) were prepared and developed as the heterogeneous Fenton-like catalysts for the removal of representative organic pollutants. Characterization results indicated that the samples with Fe₃O₄ NPs loaded outside the HNTs lumen (Fe₃O₄/HNTs) and inside the HNTs lumen (Fe₃O₄@HNTs) were successfully prepared. Both samples had typical magnetic hysteresis loops, while Fe₃O₄@HNTs exhibited higher magnetization intensity. The comparative experiments showed that Fe₃O₄@HNTs had better Fenton-like catalytic ability than that of Fe₃O₄/HNTs in the degradation of various organic pollutants. Taking Rhodamine B (RhB) as an example, the adsorption thermodynamics and kinetics of RhB onto Fe₃O₄/HNTs and Fe₃O₄@HNTs were also investigated. The comparative results demonstrated that the adsorption ability of Fe₃O₄/HNTs was better than that of Fe₃O₄@HNTs. Moreover, the dissolved concentration of Fe²⁺ and production amount of hydroxyl radical (·OH) in the Fe₃O₄@HNTs-H₂O₂ system were significantly higher than those in the Fe₃O₄/HNTs-H₂O₂ system. Based on aforementioned comparison, the nano-confinement effect in the Fe₃O₄@HNTs-H₂O₂ system was verified. This work provides meaningful guidance for the cheap and convenient design of nanoreactors for Fenton-like applications.

Keywords Fe₃O₄ halloysite nanotube adsorption Fenton-like reaction mechanism

Corresponding Author(s): Huan-Yan Xu

Issue Date: 07 February 2024

Cite this article:

Yang Li,Jia-Qi Zhou,Huan-Yan Xu, et al. Comparative studies on Fenton-like reactions catalyzed by Fe₃O₄ loaded inside and outside halloysite nanotubes for the removal of organic pollutants[J]. Front. Mater. Sci., 2024, 18(1): 240673.

URL:

https://academic.hep.com.cn/foms/EN/10.1007/s11706-024-0673-0
https://academic.hep.com.cn/foms/EN/Y2024/V18/I1/240673

Fig.1 XRD patterns of Fe₃O₄, HNTs, Fe₃O₄/HNTs and Fe₃O₄@HNTs.

Fig.2 FTIR spectra of Fe₃O₄, HNTs, Fe₃O₄/HNTs and Fe₃O₄@HNTs.

Fig.3 SEM images of (a) Fe₃O₄ NPs, (b) HNTs, (c) Fe₃O₄/HNTs, and (d) Fe₃O₄@HNTs. TEM images of (e) Fe₃O₄/HNTs and (f) Fe₃O₄@HNTs (inset: image with higher magnification).

Fig.4 Magnetization curves of Fe₃O₄/HNTs and Fe₃O₄@HNTs (insets: digital photographs of the separation of both samples by an external magnet).

Fig.5 Comparative Fenton-like degradation of (a) RhB, (b) MB, (c) MG, (d) MO, (e) CR, and (f) PNP over Fe₃O₄/HNTs and Fe₃O₄@HNTs (experimental conditions: [H₂O₂] = 3 mL·L^?1, [RhB] = [MB] = [MG] = [MO] = [CR] = [PNP] = 30 mg·L^?1, [Fe₃O₄@HNTs] = [Fe₃O₄/HNTs] = 0.5 g·L^?1, pH = 2, and T = 20 °C).

Fig.6 (a) Comparative evaluation of the RhB degradation in different systems, (b) ·OH quenching tests with 0.1 mmol·L^?1 TBA and (c) cyclic experiments (experimental conditions: [H₂O₂] = 3 mL·L^?1, [RhB] = 30 mg·L^?1, [Fe₃O₄@HNTs] = [Fe₃O₄/HNTs] = 0.5 g·L^?1, pH = 2, and T = 20 °C).

Fig.7 (a)(b) Adsorption isothermal curves, (c)(d) Langmuir fitting lines, and (e)(f) Freundlich fitting lines of RhB adsorption onto Fe₃O₄/HNTs (upper panels) and Fe₃O₄@HNTs (lower panels) (experimental conditions: pH = 2 and [Fe₃O₄/HNTs] = [Fe₃O₄@HNTs] = 0.5 g·L^?1).

Fig.8 (a)(b) Evolution of the adsorption capacity over time, (c)(d) the quasi-first-order kinetic fitting lines, and (e)(f) the quasi-second-order kinetic fitting lines of the RhB adsorption onto Fe₃O₄/HNTs and Fe₃O₄@HNTs (experimental conditions: pH = 2, [RhB] = 30 mg·L^?1, and [Fe₃O₄/HNTs] = [Fe₃O₄@HNTs] = 0.5 g·L^?1).

Tab.1 Fitting parameters of Langmuir and Freundlich models for the RhB adsorption onto Fe₃O₄/HNTs and Fe₃O₄@HNTs at different temperatures

Tab.2 Kinetic fitting parameters of quasi-first-order and quasi-second-order models

Fig.9 The evolution of reactive species in the Fe₃O₄@HNTs-H₂O₂ and Fe₃O₄/HNTs-H₂O₂ systems: (a) total iron ion concentration; (b) ferrous ion concentration; (c) absorbance of ·OH adduct; (d) H₂O₂ concentration.

Fig.10 Mechanism illustration of Fenton-like reactions catalyzed by Fe₃O₄/HNTs and Fe₃O₄@HNTs.

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