Citation: Liangbo Zhang, Jun Cheng, Yahui Shi, Kunjie Hou, Qi An, Jingyi Li, Baohui Cui, Fei Chen. Efficient removal of tetracycline hydrochloride by ZnO/HNTs composites under visible light: Kinetics, degradation pathways and mechanism[J]. Chinese Chemical Letters, ;2025, 36(7): 110400. doi: 10.1016/j.cclet.2024.110400 shu

Efficient removal of tetracycline hydrochloride by ZnO/HNTs composites under visible light: Kinetics, degradation pathways and mechanism

Liangbo Zhang ^{a, b} ,
Jun Cheng ^{a, b} ,
Yahui Shi ^{a, b} ,
Kunjie Hou ^{a, b, *,} ,
Qi An ^{a, b} ,
Jingyi Li ^{a, b} ,
Baohui Cui ^{a, b} ,
Fei Chen ^{c, *,}

a.
School of Environmental Engineering, Henan University of Technology, Zhengzhou 450001, China
b.
Henan International Joint Laboratory of Environmental Pollution, Remediation and Grain Quality Security, Zhengzhou 450001, China
c.
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China

hkj@hnu.edu.cn

fchen0505@cqu.edu.cn

Received Date: 21 May 2024
Revised Date: 14 July 2024
Accepted Date: 2 September 2024
Available Online: 3 September 2024

Figures(4)

The high band gap of zinc oxide (ZnO) has significantly limited its potential application for organic contaminant removal in photocatalysis. In this study, ZnO/halloysites (HNTs) composites (ZnO/HNTs) were prepared using a high-temperature calcination method to enhance the removal of tetracycline hydrochloride (TCH). The experimental results demonstrated that the band gap of ZnO/HNTs decreased to 3.12 eV, compared to 3.21 eV for pure ZnO. The observed removal rate (k_obs) of TCH in the ZnO/HNTs/vis system was 1.90 × 10^–2 min^-1, significantly higher than the rates in the HNTs/vis (1.25 × 10^–3 min^-1) and ZnO/vis (1.13 × 10^–2 min^-1) systems. Additionally, ZnO/HNTs exhibited strong resistance to coexisting natural organic and inorganic matter, maintaining high pollutant removal efficiency in natural water samples. The ZnO/HNTs/vis system also effectively removed other common organic pollutants, such as ciprofloxacin and methylene blue. Cycle tests indicated that the ZnO/HNTs/vis system retained 65.57% of its original efficiency, demonstrating good reusability and versatility. Scavenging and electron paramagnetic resonance experiments identified that h⁺ was the primary species in the ZnO/HNTs/vis system, with other species playing auxiliary roles in TCH degradation. This study provides valuable insights into the design of novel ZnO-based photocatalysts for the degradation of organic pollutants in water.
- Visible light,
- Tetracycline hydrochloride,
- Zinc oxide/halloysite composites,
- Mechanism
1. [1]
  D. Constantino, M.M.L. Dias, A. Silva, J.L. Faria, C.G. Silva, J. Clean. Prod. 340 (2022) 130800.
2. [2]
  F. Chen, Q. Yang, Y. Wang, et al., Chem. Eng. J. 348 (2018) 157–170.
3. [3]
  C. Sun, K.F. Zhao, A. Boies, S.N. Xiao, Z.G. Yi, Appl. Catal. B: Environ. 339 (2023) 123124.
4. [4]
  J. Zhang, J. Zhou, Mat. Sci. Semicon. Proc. 157 (2023) 107345.
5. [5]
  R. Jiang, H. Zhu, X. Zang, et al., Int. J. Biol. Macromol. 254 (2023) 127887.
6. [6]
  A.H. Bhat, N.A. Chopan, H.T.N. Chisti, Nanotechnology 34 (2023) 495604. doi: 10.1088/1361-6528/acf6c4
7. [7]
  M. Saqib, S.U. Rahman, S. Ali, et al., Mater. Today. Commun. 37 (2023) 107335.
8. [8]
  P.C. Quero Jiménez, A. Hernández Ramírez, J.L. Guzmán Mar, et al., J. Photoch. Photobio. A: Chem. 446 (2024) 115154.
9. [9]
  J. Louis, N.T. Padmanabhan, M.K. Jayaraj, H. John, Mater. Res. Bull. 169 (2024) 112542.
10. [10]
  M. Liu, D.J. ZhixinJia, C. Zhou, Prog. Polym. Sci. 39 (2014) 1498–1525.
11. [11]
  X.Y. Chen, Z.D. Zhang, S.H. Chen, et al., Opt. Mater. 134 (2022) 113202.
12. [12]
  P. Maziarz, J. Matusik, A.E. Radziszewska, J. Environ. Chem. Eng. 7 (2019) 103507.
13. [13]
  Q. Sun, Y. Sun, M. Zhou, et al., Ceram. Int. 48 (2022) 7283–7290.
14. [14]
  R. Nasser, W.B.H. Othmen, H. Elhouichet, M. Ferid, Appl. Surf. Sci. 393 (2017) 486–495.
15. [15]
  N. Kamarulzaman, M.F. Kasim, N.F. Chayed, Results Phys. 6 (2016) 217–230.
16. [16]
  J. Wang, J. Si, Y. Hao, et al., Langmuir 38 (2022) 1231–1242. doi: 10.1021/acs.langmuir.1c03024
17. [17]
  H. Cheng, Q. Liu, J. Yang, J. Zhang, R.L. Frost, Thermochim. Acta 511 (2010) 124–128.
18. [18]
  B. Zsirka, V. Vagvolgyi, E. Horvath, et al., Minerals 12 (2022) 476. doi: 10.3390/min12040476
19. [19]
  X. Gao, X. Zhang, Y. Wang, et al., Chem. Eng. J. 273 (2015) 156–165.
20. [20]
  Z. Pi, K. Hou, F. Yao, et al., Chem. Eng. J. 427 (2022) 131749.
21. [21]
  J. Guo, C.H. Shen, J. Sun, et al., Sep. Purif. Technol. 259 (2021) 118109.
22. [22]
  N. Aghababaei, M. Abdouss, H. Hosseini-Monfared, F. Ghanbari, J. Water Process. Eng. 53 (2023) 103702.
23. [23]
  Z. Shen, H. Zhou, P. Zhou, et al., J. Hazard. Mater. 425 (2021) 127781.
24. [24]
  X.J. Chen, C.W. Bai, Y. Sun, et al., Environ. Sci. Technol. 57 (2023) 20206–20218. doi: 10.1021/acs.est.3c06370
25. [25]
  F. Chen, Y. Sun, X. Huang, et al., Proc. Natl. Acad. Sci. U. S. A. 124 (2024) 2314396121.
26. [26]
  J. Wu, T. Yang, F. Chen, H. Yu, PNAS Nexus 3 (2024) 1–10.
27. [27]
  M. Preeyanghaa, A. Ilamparidhi, J. Madhavan, B. Neppolian, Chemosphere 303 (2022) 135070.
28. [28]
  D. Qiao, Z. Li, J. Duan, X. He, Chem. Eng. J. 400 (2020) 125952.
29. [29]
  C. Wu, H. Zuo, H. Du, et al., Sep. Purif. Technol. 282 (2022) 120096.
30. [30]
  X. Gu, R. Xu, G. Yuan, et al., Anal. Chim. Acta 675 (2010) 64–70.
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  Teng Wang , Jiachun Cao , Juan Li , Didi Li , Zhimin Ao . A novel photocatalytic mechanism of volatile organic compounds degradation on BaTiO₃ under visible light: Photo-electrons transfer from photocatalyst to pollutant. Chinese Chemical Letters, 2025, 36(3): 110078-. doi: 10.1016/j.cclet.2024.110078
13. [13]
  Ruiheng Liang , Huizhong Wu , Zhongzheng Hu , Ge Song , Xuyang Zhang , Omotayo A. Arotiba , Minghua Zhou . Hierarchical Fe-Bi/Bi₇O₉I₃/OVs microspheres coupled with natural air diffusion electrode to achieve efficient heterogeneous visible-light-driven photoelectro-Fenton degradation of tetracycline without aeration. Chinese Chemical Letters, 2025, 36(4): 110136-. doi: 10.1016/j.cclet.2024.110136
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  Xin Li , Wanting Fu , Ruiqing Guan , Yue Yuan , Qinmei Zhong , Gang Yao , Sheng-Tao Yang , Liandong Jing , Song Bai . Nucleophiles promotes the decomposition of electrophilic functional groups of tetracycline in ZVI/H₂O₂ system: Efficiency and mechanism. Chinese Chemical Letters, 2024, 35(10): 109625-. doi: 10.1016/j.cclet.2024.109625
15. [15]
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16. [16]
  Tong Zhou , Liyi Xie , Chuyu Liu , Xiyan Zheng , Bao Li . Between Sobriety and Intoxication: The Fascinating Journey of Sauce-Flavored Latte. University Chemistry, 2024, 39(9): 55-58. doi: 10.12461/PKU.DXHX202312048
17. [17]
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