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. 2024 Jun 1;22(2):483-501.
doi: 10.1007/s40201-024-00906-0. eCollection 2024 Dec.

Ultrasound-assisted heterogeneous process for organic dye pollutants destruction using the novel MIL-101(Fe)/ZrO2/MnFe2O4 nanocomposite catalyst from water medium

Meysam Sadeghi  1 , Pourya Zarshenas  2
Affiliations

Ultrasound-assisted heterogeneous process for organic dye pollutants destruction using the novel MIL-101(Fe)/ZrO2/MnFe2O4 nanocomposite catalyst from water medium

Meysam Sadeghi et al. J Environ Health Sci Eng. .

Abstract

The heterogeneous sonocatalysis is considered as an impressive remediation approach to eliminate the dyeing wastewaters. Among the efficient sonocatalytic remediation, nanocomposite sonocatalysts have grabbed special attention in recent years. In the presence research, the novel MIL-101(Fe)/ZrO2/MnFe2O4 nanocomposite as a magnetically retrievable catalyst was elaborated using the ultrasound-assisted hydrothermal route and its sonocatalytic performance was tested applying the methylene blue (MB), rhodamine B (RhB), congo red (CR), and methyl orange (MO) organic dyes under US/H2O2 system. The as-fabricated nanocomposite is well identified via FESEM, TEM, EDX, EDX elemental dot mappings, AFM, FTIR, XRD, BET, UV-Vis DRS, and VSM. The sonocatalytic destruction outcomes have demonstrated that the MIL-101(Fe)/ZrO2/MnFe2O4 shows appreciable performance for the destruction of MB, RhB, CR, and MO with the yields of 98.17%, 96.35%, 93.40%, and 89.82%, respectively under the optimized conditions of irradiation time of 7 min, dye concentration of 25 mg/L, catalyst amount of 10 mg, US power intensity of 100 W, H2O2 concentration of 4 mM, pH of 7, and temperature of 25 ± 1 °C. The fitted kinetic curves were exhibited a first-order model and the half-life time (t1/2) and reaction rate constant (kapp) of the MB sonodestruction were determined to be 1.20 min and 0.5768 min-1 employing the MIL-101(Fe)/ZrO2/MnFe2O4/US/H2O2 system, respectively. The free •OH radicals were having a crucial role in the MB sonodestruction reaction, affirmed via quenching the experiments. Besides, the reusing experiments indicate that the MIL-101(Fe)/ZrO2/MnFe2O4 represents propitious stability and long durability and reminded more than 93% after four cycles.

Graphical abstract: The metal-organic framework MIL-101(Fe)/ZrO2/MnFe2O4 heterojunction magnetically retrievable nanocomposite was successfully prepared and used as a new sonocatalyst for the destruction of MB, RhB, CR, and MO toxic organic dye pollutants from water medium.

Keywords: Heterogeneous sonocatalysis; Kinetic; MIL-101(Fe)/ZrO2/MnFe2O4; Organic dye; Ultrasound-assisted hydrothermal.

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Conflict of interest statement

Competing interestsThe authors declare no competing interests.

Figures

Scheme 1
Scheme 1
The preparation pathway of the MIL-101(Fe)/ZrO2/MnFe2O4 nanocomposite
Fig. 1
Fig. 1
FESEM micrographs of: (a) MIL-101(Fe), (b) MIL-101(Fe)/ZrO2/MnFe2O4, (c) ZrO2 and (d) MnFe2O4. (e) and (f) TEM micrographs of the MIL-101(Fe)/ZrO2/MnFe2O4.
Fig. 2
Fig. 2
EDX spectra of: (a) MIL-101(Fe), (b) MIL-101(Fe)/ZrO2/MnFe2O4 and (c) EDX micrograph elemental dot mappings of the MIL-101(Fe)/ZrO2/MnFe2O4.
Fig. 3
Fig. 3
(a) and (b) 2D and 3D AFM micrographs of the MIL-101(Fe)/ZrO2/MnFe2O4.
Fig. 4
Fig. 4
FTIR spectra of: (a) MIL-101(Fe), (b) MIL-101(Fe)/ZrO2/MnFe2O4, (c) ZrO2, and (d) MnFe2O4.
Fig. 5
Fig. 5
XRD patterns of: (a) MIL-101(Fe), (b) MIL-101(Fe)/ZrO2/MnFe2O4, (c) ZrO2, and (d) MnFe2O4.
Fig. 6
Fig. 6
(a) and (b) BET-BJH analysis of the MIL-101(Fe)/ZrO2/MnFe2O4. (c) UV-Vis DRS analysis of the as-prepared sonocatalysts and (d) VSM curves of: (I) MnFe2O4 and (II) MIL-101(Fe)/ZrO2/MnFe2O4.
Fig. 7
Fig. 7
The dark adsorption-desorption equilibrium of the MB on different catalysts versus the irradiation time (a), UV-Vis absorption spectra changes of the MB sonodestruction over the MIL-101(Fe)/ZrO2/MnFe2O4 versus the irradiation time (b and c), and the first-order kinetic curve (ln(C0/Ct)) versus the irradiation time (d), (optimized conditions; [MB]o: 25 mg/L (50 mL), [H2O2]: 4 mM (2 mL), MIL-101(Fe)/ZrO2/MnFe2O4 amount: 10 mg, US power intensity: 100 W, pH = 7, and temperature: 25 ± 1 °C)
Fig. 8
Fig. 8
The effects of: (a) initial MB concentration, (b) H2O2 concentration, (c) MIL-101(Fe)/ZrO2/MnFe2O4 amount, (d) US power intensity, and (e) solution pH on the MB sonodestruction by the MIL-101(Fe)/ZrO2/MnFe2O4.
Fig. 9
Fig. 9
UV-Vis absorption spectra of: (a) RhB and (b) MO versus the irradiation time. (c) Sonodestruction efficiency% versus the organic dye type on the MIL-101(Fe)/ZrO2/MnFe2O4 (optimized conditions; [dye]o: 25 mg/L (50 mL), [H2O2]: 4 mM (2 mL), MIL-101(Fe)/ZrO2/MnFe2O4 amount: 10 mg, US power intensity: 100 W, pH = 7, and temperature: 25 ± 1 °C)
Scheme 2
Scheme 2
The plausible mechanism allocated to the dyes sonodestruction (a) Type-II, and Z-scheme pathways over the MIL-101(Fe)/ZrO2/MnFe2O4/US/H2O2 system from water media
Fig. 10
Fig. 10
Total organic carbon (TOC) in the sonodestruction of organic dyes on the MIL-101(Fe)/ZrO2/MnFe2O4.
Fig. 11
Fig. 11
(a) PL spectra of: (I) ZrO2 and (II) MIL-101(Fe)/ZrO2/MnFe2O4, (b) PL spectra of TPA reagent on the MB sonodestruction over the MIL-101(Fe)/ZrO2/MnFe2O4/US/H2O2 system, (c) The impact of the quencher type over the MB sonodestruction on the MIL-101(Fe)/ZrO2/MnFe2O4. (d) The regeneration curve and (e) TEM analysis of the recovered MIL-101(Fe)/ZrO2/MnFe2O4 over the MB sonodestruction after four cycles
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