INVESTIGATION OF Mn-DOPED LAYERED DOUBLE HYDROXIDE CATALYSTS FOR THE TREATMENT OF METHYLENE BLUE-CONTAMINATED WASTEWATER

Authors

  • Trần Bảo Châu
  • Nguyễn Phan Trúc Xuyên
  • Cáp Hải Minh Nguyên
  • Huỳnh Thị Phương Nhung
  • Võ Châu Ngọc Anh
  • Đỗ Mai Nguyễn
  • Nguyễn Vũ Bảo Chi
  • Nguyễn Khoa Thị Phượng
  • Hoàng Hiền Ý
  • Đào Anh Quang

Keywords

Mn–Mg–Al LDH, Advanced oxidation processes, Methylene blue removal, Catalytic oxidation, Bicarbonate activated hydrogen peroxide, Quá trình oxy hóa nâng cao, Xử lý xanh methylen, Oxy hóa xúc tác, Hydroperoxit hoạt hóa bicacbonat

DOI:

https://doi.org/10.34238/tnu-jst.13846

Abstract

In this study, Mg–Al layered double hydroxides modified with manganese nanoparticles were successfully synthesized via a co-precipitation route and subsequently evaluated for their catalytic performance in the degradation of methylene blue. The structural and morphological characteristics of the synthesized materials were thoroughly characterized using X-ray diffraction and scanning electron microscopy, which confirmed the successful synthesis of the investigated material. The effect of varying manganese nanoparticle loadings on the catalytic efficiency was systematically investigated using an advanced oxidation system comprising bicarbonate and hydrogen peroxide. Among the different formulations tested, the material prepared with a molar ratio of Mg:Al:Mn = 0.15:0.05:12.5×10−4 exhibited the highest removal efficiency, achieving over 90% degradation of methylene blue within 35 minutes. Additionally, the catalyst demonstrated remarkable stability, maintaining consistent performance across at least six consecutive reaction cycles. The catalytic role of manganese-modified Mg–Al layered double hydroxides is clearly demonstrated by the experimental results obtained in this study, indicating their strong potential for application in the treatment of wastewater containing organic dyes from the textile dyeing industry.

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References

E. O. Atakpa et al., “Hybrid layered double hydroxide–bacteria systems for wastewater treatment: Toward tunable bio-inorganic interfaces and environmental remediation,” Sci. Total Environ., vol. 1002, 2025, Art. no. 180575.

L. Li et al., “A systematic review on percarbonate-based advanced oxidation processes in wastewater remediation: From theoretical understandings to practical applications,” Water Res., vol. 259, 2024, Art. no. 121842.

L. Ge et al., “Layered double hydroxide based materials applied in persulfate based advanced oxidation processes: Property, mechanism, application and perspectives,” J. Hazard. Mater., vol. 424, 2022, Art. no. 127612.

A. E. Gahrouei, S. Vakili, A. Zandifar, and S. Pourebrahimi, “From wastewater to clean water: Recent advances on the removal of metronidazole, ciprofloxacin, and sulfamethoxazole antibiotics from water through adsorption and advanced oxidation processes (AOPs),” Environ. Res., vol. 252, 2024, Art. no. 119029.

A. Faggiano, A. B. Martínez-Piernas, M. Ricciardi, O. Motta, A. Fiorentino, and A. Proto, “A chemometric approach to the interaction of hydrogen peroxide and thermally activated persulfate in the removal of aromatic compounds,” J. Environ. Manage., vol. 373, 2025, Art. no. 123957.

H. Pan, Y. Gao, N. Li, Y. Zhou, Q. Lin, and J. Jiang, “Recent advances in bicarbonate-activated hydrogen peroxide system for water treatment,” Chem. Eng. J., vol. 408, 2021, Art. no. 127332.

G. Zhang et al., “Freezing-enhanced degradation of naproxen by bicarbonate activated hydrogen peroxide: Peformance and mechanisms,” Chem. Eng. J., vol. 514, Jun. 2025, Art. no. 163373.

A. Jawad, Z. Chen, and G. Yin, “Bicarbonate activation of hydrogen peroxide: A new emerging technology for wastewater treatment,” Chinese J. Catal., vol. 37, no. 6, pp. 810–825, 2016.

W. Zhang et al., “Vacancy-strengthened Cu/Co composite oxides for efficient removal of methylene blue via peroxymonosulfate activation: Synergism of multiple Lewis acid sites,” J. Environ. Chem. Eng., vol. 12, no. 5, 2024, Art. no. 113889.

A. Sharmin, G. Zhang, M. A. Bhuiyan, and B. K. Pramanik, “A high-flux atomically dispersed MIL-100 (Fe) incorporated PMS-based LDH catalytic membrane for the removal of micropollutants from secondary effluent wastewater,” Chem. Eng. J., vol. 495, 2024, Art. no. 153572.

G. Radji, N. Bettahar, A. Bahmani, I. Boukhetache, and S. Contreras, “Heterogeneous Fenton-like degradation of organic pollutants in petroleum refinery wastewater by copper-type layered double hydroxides,” J. Water Process Eng., vol. 50, 2022, Art. no. 103305.

J. Rui et al., “Activation of persulfate via Mn doped Mg/Al layered double hydroxide for effective degradation of organics: Insights from chemical and structural variability of catalyst,” Chemosphere, vol. 302, 2022, Art. no. 134849.

M. Samandari, A. T. Manesh, S. A. Hosseini, and S. Mansouri, “Mg-Al LDH and calcined LDH: Green nanocatalysts for wet peroxide oxidation of phenol in wastewater,” J. Water Environ. Nanotechnol., vol. 6, no. 1, pp. 72–80, 2021.

K. Warmuz and D. Madej, “Synthesis and evaluation of Mg-Al hydrotalcite formation and its influence on the microstructural evolution of spinel-forming refractory castables under intermediate temperatures,” J. Eur. Ceram. Soc., vol. 42, no. 5, pp. 2545–2555, 2022.

Heriyanto, E. Heraldy, and K. D. Nugrahaningtyas, “X-RAY Diffraction and Fourier Transform Infrared Study of Ca-Mg-Al Hydrotalcite from Artificial Brine Water with Synthesis Hydrothermal Treatments,” IOP Conf. Ser. Mater. Sci. Eng., vol. 333, 2018, Art. no. 012006.

Y. Hanifah, R. Mohadi, M. Mardiyanto, N. Ahmad, S. Suheryanto, and A. Lesbani, “Polyoxometalate Intercalated M2+/Al (M2+=Ni, Mg) Layered Double Hydroxide for Degradation of Methylene Blue,” Bull. Chem. React. Eng. Catal., vol. 18, no. 2, pp. 210–221, 2023.

H. T. Berede et al., “Photocatalytic activity of the biogenic mediated green synthesized CuO nanoparticles confined into MgAl LDH matrix,” Sci. Rep., vol. 14, no. 1, Jan. 2024, Art. no. 2314.

K. G. Omdeo et al., “Surface Modification of Synthesized Layered Double Hydroxide [LDH] for Methylene Blue Dye Removal in Textile Industry via Photocatalytic Activity under Visible Light,” J. Nano Res., vol. 46, pp. 135–147, 2017.

R. H. Al-Ammari, S. D. Al-Malwi, M. A. Abdel-Fadeel, S. M. Bawaked, and M. M. M. Mostafa, “Zn-Layered Double Hydroxide Intercalated with Graphene Oxide for Methylene Blue Photodegradation and Acid Red Adsorption Studies,” Catalysts, vol. 14, no. 12, 2024, doi: 10.3390/catal14120897.

Q. Li, X. Jiang, and Y. Lian, “The Efficient Photocatalytic Degradation of Organic Pollutants on the MnFe2O4/BGA Composite under Visible Light,” Nanomaterials, vol. 11, no. 5, 2021, doi: 10.3390/nano11051276.

J. J. Pignatello, E. Oliveros, and A. MacKay, “Advanced Oxidation Processes for Organic Contaminant Destruction Based on the Fenton Reaction and Related Chemistry,” Crit. Rev. Environ. Sci. Technol., vol. 36, no. 1, 2006, doi: 10.1080/10643380500326564.

N. A. Urbina-Suarez, C. Rivera-Caicedo, Á. D. González-Delgado, A. F. Barajas-Solano, and F. Machuca-Martínez, “Bicarbonate-Hydrogen Peroxide System for Treating Dyeing Wastewater: Degradation of Organic Pollutants and Color Removal,” Toxics, vol. 11, no. 4, 2023, doi: 10.3390/toxics11040366.

B. Li et al., “Complexation between butyl xanthate and Cu enhanced peroxydisulfate activation and cation redox cycle by Fe-Cu-LDH/biochar,” J. Environ. Chem. Eng., vol. 12, no. 2, 2024, Art. no. 112466.

R. Ma et al., “Decoding the entropy-stabilized matrix of high-entropy layered double hydroxides: Harnessing strain dynamics for peroxymonosulfate activation and tetracycline degradation,” J. Colloid Interface Sci., vol. 680, pp. 676–688, 2025.

Published

2025-12-15

Issue

Section

NATURAL SCIENCE – ENGINEERING – TECHNOLOGY