Abstract
Semiconductor photocatalysis is a green and environmentally friendly antibiotic wastewater treatment technology without secondary pollution. In this paper, a series of montmorillonite (MMT) samples loaded with Cu, Mn, and Ni were prepared by impregnation method. The structure and spectral response of the as-prepared samples were characterized by powder X-ray diffraction, energy-dispersive spectroscopy, laser Raman spectroscopy, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, UV–Vis diffuse reflectance spectroscopy (UV–Vis DRS), electrochemical impedance spectroscopy, and photocurrent response test. The photocatalytic degradation of tetracycline hydrochloride (TCH) was carried out under simulated solar irradiation, and the photocatalytic properties of MMT samples with different loads were investigated. The characterization results show that Cu and Mn have strong interaction with MMT, and composite photocatalyst Cu10Mn10-MMT has the smallest Nyquist arc and higher photocurrent intensity. Degradation experiments on TCH showed that Cu10Mn10-MMT had the best photocatalytic degradation, with a degradation rate of 79.78%, three times that of the original MMT. Active substances capture experiments showed that h+ and O2.− were the main active substances for the degradation of TCH by Cu10Mn10-MMT. After the combination of Cu, Mn, and MMT, the band structure changed, resulting in more h+ and O2.− involved in the redox reaction, thereby improving the photocatalytic degradation performance of TCH. In this work, a promising photocatalyst is used to efficiently and greenly degrade antibiotic wastewater.
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References
A.A. Anthony, C.F. Adekunle, A.S. Thor, Residual antibiotics, antibiotic resistant superbugs and antibiotic resistance genes in surface water catchments: Public health impact. Phys. Chem. Earth Parts A/B/C 105, 177–183 (2018)
D. Fabregat-Safont, E. Gracia-Marín, M. Ibáñez et al., Analytical key issues and challenges in the LC-MS/MS determination of antibiotics in wastewater. Anal. Chim. Acta. 1239, 340739 (2023)
F. Ahmad, D. Zhu, J. Sun, Environmental fate of tetracycline antibiotics: degradation pathway mechanisms, challenges, and perspectives. Environ. Sci. Eur. 33, 64 (2021)
C. Lv, X. Lan, L. Wang et al., Rapidly and highly efficient degradation of tetracycline hydrochloride in wastewater by 3D IO–TiO2–CdS nanocomposite under visible light. Environ. Technol. 42, 377–387 (2021)
B.H. Diya’uddeen, A.R. Abdul Aziz, W.M. Daud, On the limitation of Fenton oxidation operational parameters: a review. Int. J. Chem. Reactor Eng. (2012). https://doi.org/10.1515/1542-6580.2913
K. Awaya, K. Hatakeyama, M. Koinuma et al., Surface state change effects of electrochemically oxidized/reduced glassy carbon on electrochemical capacitance. Chem. Lett. 46, 1030–1032 (2017)
R. Pandiselvam, M.R. Manikantan, V. Divya et al., Ozone: an advanced oxidation technology for starch modification. Ozone 41, 491–507 (2019)
Y. Shi, Z. Yan, Y. Xu et al., Visible-light-driven AgBr–TiO2-Palygorskite photocatalyst with excellent photocatalytic activity for tetracycline hydrochloride. J. Clean. Prod. 277, 124021 (2020)
Y. Shi, J. Li, D. Wan et al., Peroxymonosulfate-enhanced photocatalysis by carbonyl-modified g-C3N4 for effective degradation of the tetracycline hydrochloride. Sci. Total Environ. 749, 142313 (2020)
F.S. Freyria, M. Armandi, M. Compagnoni et al., Catalytic and photocatalytic processes for the abatement of N-containing pollutants from wastewater. Part 2: organic pollutants. J. Nanosci. Nanotechnol. 17, 3654–3672 (2017)
S.-L. Bee, M.A.A. Abdullah, S.-T. Bee et al., Polymer nanocomposites based on silylated-montmorillonite: a review. Progr. Polym. Sci. 85, 57–82 (2018)
O.V. Alekseeva, A.N. Rodionova, N.A. Bagrovskaya et al., Synthesis, structure, and properties of a bentonite–magnetite composite. Prot. Met. Phys. Chem. 52, 819–824 (2016)
W. Mulewa, M. Tahir, N.A.S. Amin, MMT-supported Ni/TiO2 nanocomposite for low temperature ethanol steam reforming toward hydrogen production. Chem. Eng. J. 326, 956–969 (2017)
L. Yang, Q. Wang, J.R. Rangel-Mendez et al., Self-assembly montmorillonite nanosheets supported hierarchical MoS2 as enhanced catalyst toward methyl orange degradation. Mater. Chem. Phys. 246, 122829 (2020)
P. Pannak, A. Songsasen, W. Foytong et al., Homogeneous distribution of nanosized ZnO in montmorillonite clay sheets for the photocatalytic enhancement in degradation of Rhodamine B. Res. Chem. Intermed. 44, 6861–6875 (2018)
D. Yang, J. Chen, X. Hong et al., One-pot synthesis of TiO2/hectorite composite and its photocatalytic degradation of methylene blue. Catalysts 12, 297 (2022)
A.L. Utz, Vibrations that live long and prosper. Nat. Chem. 10, 577–578 (2018)
A. Garg, M. Milina, M. Ball et al., Transition-metal nitride core@noble-metal shell nanoparticles as highly CO tolerant catalysts. Angew. Chem. Int. Ed. 56, 8828–8833 (2017)
H. Yi, T. Tao, S. Zhao et al., Promoted adsorption of methyl mercaptan by γ-Al2O3 catalyst loaded with Cu/Mn. Environ. Technol. Innovation. 21, 101349 (2021)
H. Jouini, I. Mejri, J. Martinez-Ortigosa et al., Selective catalytic reduction of nitric oxide with ammonia over Fe–Cu modified highly silicated zeolites. Solid State Sci. 84, 75–85 (2018)
F. Liu, H. Zhang, Y. Yan et al., Preparation and characterization of Cu and Mn modified beta zeolite membrane catalysts for toluene combustion. Mater. Chem. Phys. 241, 122322 (2020)
Q.-C. Yu, S.-C. Zhang, B. Yang, Dispersion of copper oxide supported on γ-alumina and its sulfation properties. Trans. Nonferrous Met. Soc. China 21, 2644–2648 (2011)
S. Sohrabnezhad, A. Pourahmad, T. Salavatiyan, CuO–MMT nanocomposite: effective photocatalyst for the discoloration of methylene blue in the absence of H2O2. Appl. Phys. A 122, 111 (2016)
O. Diachenko, J. Kováč, O. Dobrozhan et al., Structural and optical properties of CuO thin films synthesized using spray pyrolysis method. Coatings 11, 1392 (2021)
A.A. Dubale, I.N. Ahmed, Y.-J. Zhang et al., A facile strategy for fabricating C@Cu2O/CuO composite for efficient photochemical hydrogen production with high external quantum efficiency. Appl. Surf. Sci. 534, 147582 (2020)
K. Mohamed Racik, A. Manikandan, M. Mahendiran et al., Fabrication of manganese oxide decorated copper oxide (MnO2/CuO) nanocomposite electrodes for energy storage supercapacitor devices. Physica E. 119, 114033 (2020)
J. Yin, Y. Li, F. Lv et al., Oxygen vacancies dominated NiS2/CoS2 interface porous nanowires for portable Zn–air batteries driven water splitting devices. Adv. Mater. 29, 1704681 (2017)
D. Xu, B. Cheng, S. Cao et al., Enhanced photocatalytic activity and stability of Z-scheme Ag2CrO4-GO composite photocatalysts for organic pollutant degradation. Appl. Catal. B 164, 380–388 (2015)
Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (Grant No. 21271008) and the Anhui Provincial Natural Science Foundation (Grant No. 2008085QE194), Research Foundation of the Institute of Environment-friendly Materials and Occupational Health of Anhui University of Science and Technology (Wuhu) (Grant Nos. ALW2020YF01, ALW2020YF09).
Funding
Funding was provided by the National Natural Science Foundation of China (Grant No. 21271008), the Anhui Provincial Natural Science Foundation (Grant No. 2008085QE194), Environmentally Friendly Materials and Occupational Health Research Institute, Anhui University of Science and Technology (Grant Nos. ALW2020YF01, ALW2020YF09).
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LH contributed to experiments, characterization, data analysis, and writing—original draft. KY contributed to conceptualization, data curation, formal analysis, writing—review and editing. XL contributed to characterization work and mechanism analysis work. JZ contributed to data analysis and investigation. JH contributed to academic guidance, writing—review and editing. XC contributed to writing—review and editing.
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Hu, L., Yang, K., Liu, X. et al. Promoted photocatalytic degradation of tetracycline hydrochloride by montmorillonite catalyst loaded with Cu/Mn. J Mater Sci: Mater Electron 34, 1471 (2023). https://doi.org/10.1007/s10854-023-10862-4
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DOI: https://doi.org/10.1007/s10854-023-10862-4