Citation: Ping ZHANG, Chenchen ZHAO, Xiaoyun CUI, Bing XIE, Yihan LIU, Haiyu LIN, Jiale ZHANG, Yu'nan CHEN. Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides[J]. Chinese Journal of Inorganic Chemistry, ;2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014 shu

Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides

1.
School of Resources and Environment, Nanchang University, Nanchang 330031, China
2.
Center of Analysis and Testing, Nanchang University, Nanchang 330031, China
3.
School of Physics and Materials Science, Nanchang University, Nanchang 330031, China

Corresponding author: Bing XIE, zhangping@ncu.edu.cn
Received Date: 11 January 2024
Revised Date: 22 July 2024

Figures(9)

The precursor-calcination approach was employed to fabricate ZnAl@layered double oxides (LDOs) with dual functionality with adsorption and photocatalysis. The effect of bimetallic ratios and calcination temperatures on the adsorption-photocatalytic degradation of tetracycline (TC) was systematically investigated by X-ray powder diffraction (XRD), infrared spectroscopy (FTIR), ultraviolet-visible diffuse reflection spectroscopy (UV-Vis DRS), and scanning electron microscope (SEM). The results indicated that a molar ratio of 2∶1 for Zn to Al and a calcination temperature of 400 ℃ resulted in Zn₂Al₁@LDO₄₀₀ with outstanding adsorption-photocatalytic activity. Moreover, adsorption studies revealed that Zn₂Al₁@LDO₄₀₀ displayed the chemisorption-limited heterogeneous monolayer adsorption for TC, with higher temperatures promoting the adsorption process. Simultaneously, the collaborative degradation of TC by photogenerated holes (h⁺), hydroxyl radicals (·OH), and superoxide radicals (·O₂^-) was confirmed through free radical quenching experiments and electron paramagnetic resonance (EPR) tests.
- layered double oxide,
- tetracycline,
- adsorption-photocatalytic,
- collaborative degradation
1. [1]
  Shao S C, Wu X W. Microbial degradation of tetracycline in the aquatic environment: A review. Crit. Rev. Biotechnol., 2020, 40(7): 1010-1018 doi: 10.1080/07388551.2020.1805585
2. [2]
  Zhang Z, Chen Y, Wang P, Wang Z, Zuo C, Chen W Q, Ao T Q. Facile fabrication of N-doped hierarchical porous carbons derived from soft-templated ZIF-8 for enhanced adsorptive removal of tetracycline hydrochloride from water. J. Hazard. Mater., 2022, 423: 127103 doi: 10.1016/j.jhazmat.2021.127103
3. [3]
  Xiong W P, Zeng Z T, Zeng G M, Yang Z, Xiao R, Li X, Cao J, Zhou C, Chen H, Jia M, Yang Y, Wang W, Tang X. Metal-organic frameworks derived magnetic carbon-αFe/Fe₃C composites as a highly effective adsorbent for tetracycline removal from aqueous solution. Chem. Eng. J., 2019, 374: 91-99 doi: 10.1016/j.cej.2019.05.164
4. [4]
  MAO J Y, HUANG Y W, HUANG Z Q, LIU X P, XUE H, XIAO L R. Different photocatalytic performances for tetracycline hydrochloride degradation of p-block metal oxides Ga₂O₃ and Sb₂O₃. Chinese J. Inorg. Chem., 2021, 37(3): 509-515 doi: 10.11862/CJIC.2021.063
5. [5]
  Rodriguez-Mozaz S, Chamorro S, Marti E, Huerta B, Gros M, Sànchez-Melsió A, Borrego C M, Barceló D, Balcázar J L. Occurrence of antibiotics and antibiotic resistance genes in hospital and urban wastewaters and their impact on the receiving river. Water Res., 2015, 69: 234-242 doi: 10.1016/j.watres.2014.11.021
6. [6]
  Dong W Y, Cai T, Liu Y T, Wang L L, Chen H, Zeng W G, Li J, Li W L. Rapid removal of organic pollutants by a novel persulfate-brochantite system: Mechanism and implication. J. Colloid Interface Sci., 2021, 585: 400-407 doi: 10.1016/j.jcis.2020.11.106
7. [7]
  ZHANG X X, NIU Y Y. Synthesis of metal coordination compounds containing benzimidazole tripod ligand and their adsorption properties for iodine. Chinese J. Inorg. Chem., 2024, 40(1): 111-123 doi: 10.11862/CJIC.20230335
8. [8]
  Samuel O, Francis O, Penny P. Tuning the electronic and structural properties of Gd-TiO₂-GO nanocomposites for enhancing photodegradation of IC dye: The role of Gd³⁺ ion. Appl. Catal. B-Environ., 2019, 243, 106-120 doi: 10.1016/j.apcatb.2018.10.031
9. [9]
  LIU P, ZHU C C, LI Y Y, YAO H C. Construction and photocatalytic CO₂ reduction performance of S-scheme heterojunction ZnFe₂O₄/WO₃ catalysts. Chinese J. Inorg. Chem., 2024, 40(1): 197-208 doi: 10.11862/CJIC.20230376
10. [10]
  Chandrasekaran S, Bowen C, Zhang P X, Li Z L, Yuan Q H, Ren X Z, Deng L B. Spinel photocatalysts for environmental remediation, hydrogen generation, CO₂ reduction and photoelectrochemical water splitting. J. Mater. Chem. A, 2018, 6: 11078-11104 doi: 10.1039/C8TA03669A
11. [11]
  Ahmed A, Talib Z, Hussein M, Zakaria A. Improvement of the crystallinity and photocatalytic property of zinc oxide as calcination product of Zn-Al layered double hydroxide. J. Alloy. Compd., 2012, 539: 154-160 doi: 10.1016/j.jallcom.2012.05.093
12. [12]
  Rodriguez-Rivas F, Pastor A, Barriga C, Cruz-Yusta M, Sánchez L, Pavlovic I. Zn-Al layered double hydroxides as efficient photocatalysts for NOx abatement. Chem. Eng. J., 2018, 346: 151-158 doi: 10.1016/j.cej.2018.04.022
13. [13]
  Xia S J, Liu F X, Ni Z M, Xue J L, Qian P P. Layered double hydroxides as efficient photocatalysts for visible-light degradation of rhodamine B. J. Colloid Interface Sci., 2013, 405: 195-200 doi: 10.1016/j.jcis.2013.05.064
14. [14]
  Suárez-Quezada M, Romero-Ortiz G, Samaniego-Benítez J, Suárez V, Mantilla A. H₂ production by the water splitting reaction using photocatalysts derived from calcined ZnAl LDH. Fuel, 2019, 240: 262-269 doi: 10.1016/j.fuel.2018.11.155
15. [15]
  Cao Y, Li G T, Li X B. Graphene/layered double hydroxide nanocomposite: Properties, synthesis, and applications. Chem. Eng. J., 2016, 292: 207-223 doi: 10.1016/j.cej.2016.01.114
16. [16]
  Wang F H, Liu X Z, Xu L, Zheng X G. One-pot synthesis of CeO₂/ Mg-Al layered double oxide nanosheets for efficient visible-light-induced photo-reduction of Cr(Ⅵ). Colloids Surf. A-Physicochem. Eng. Asp., 2020, 601: 125044 doi: 10.1016/j.colsurfa.2020.125044
17. [17]
  Zhu D Y, Xue S K, Yang S F, Zuo Q, Wang H Y, Lu Q J, Ruan G H, Zhao C X, Du F Y. Layered bimetallic oxide composite film: A highly efficient and reusable photocatalytic film for removal of tetracycline antibiotics. Chem. Eng. J., 2023, 476: 146681 doi: 10.1016/j.cej.2023.146681
18. [18]
  Wu H, Liu X Z, Wen J, Liu Y, Zheng X G. Rare-earth oxides modified Mg-Al layered double oxides for the enhanced adsorption-photocatalytic activity. Colloids Surf. A-Physicochem. Eng. Asp., 2021, 610: 125933 doi: 10.1016/j.colsurfa.2020.125933
19. [19]
  Zhang X Y, Dai B S, Ren S C, Hu Z N, Zheng X, Wang Y, Sun H B, Niu D, Wang L S. Iron diffusion-doped magnesium-aluminum layered double oxides as a multifunctional adsorbent for removal of F, Sb(Ⅲ) and methyl orange contaminants from water. Korean J. Chem. Eng., 2020, 37(5): 792-803 doi: 10.1007/s11814-020-0487-4
20. [20]
  Suwanboon S, Amornpitoksuk P, Rattana T, Randorn C. Investigation of g-C₃N₄/ZnAl₂O₄ and ZnO/ZnAl₂O₄ nanocomposites: From synthesis to photocatalytic activity of pollutant dye model. Ceram. Int., 2020, 46(14): 21958-21977 doi: 10.1016/j.ceramint.2020.04.243
21. [21]
  FU Y P, YANG H, QIAO D, DONG L L, CHEN X L, CUI H L, LIU L, WANG J J. Synthesis, crystal structure, and photocatalytic activity of Co(Ⅱ) and Ni(Ⅱ) complexes based on pyromellitic acid and bis (imidazole)methyl benzene. Chinese J. Inorg. Chem., 2023, 39(12): 2393-2406 doi: 10.11862/CJIC.2023.200
22. [22]
  Ji F, Li J, Cui X L, Liu J, Bing X M, Song P. Hierarchical C-doped BiPO₄/ZnCoAl-LDO hybrid with enhanced photocatalytic activity for organic pollutants degradation. Appl. Clay Sci., 2018, 162: 182-191 doi: 10.1016/j.clay.2018.06.012
23. [23]
  Yuan Z J, Bak S, Li P S, Jia Y, Zheng Li R, Zhou Y, Bai L, Hu E Y, Yang X, Cai Z, Sun Y M, Sun X M. Activating layered double hydroxide with multivacancies by memory effect for energy-efficient hydrogen production at neutral pH. ACS Energy Lett., 2019, 4(6): 1412-1418 doi: 10.1021/acsenergylett.9b00867
24. [24]
  Martino A, Arienzo M, Iorio M, Vinale F, Lorito M, Prenzler P, Ryan D, Obied H. Detoxification of olive mill wastewaters by zinc-aluminum layered double hydroxides. Appl. Clay Sci., 2011, 53(4): 737-744 doi: 10.1016/j.clay.2011.07.003
25. [25]
  Deng Y, Li K, Guan Q Q, Hu T D, He L. Novel CNFs-based organic UV-adsorber intercalated ZnAl-LDHs composited films with superior photothermal stability and mechanical properties. Ind. Crops Prod., 2022, 178: 114555 doi: 10.1016/j.indcrop.2022.114555
26. [26]
  Fahoul Y, Zouheir M, Tanji K, Kherbeche A. Synthesis of a novel ZnAl₂O₄/CuS nanocomposite and its characterization for photocatalytic degradation of acid red 1 under UV illumination. J. Alloy. Compd., 2021, 889: 161708 doi: 10.1016/j.jallcom.2021.161708
27. [27]
  Cao M B, Liu X, Wang W, Gao M, Li Y S, Yang H B. Functionalized Zn/Al N-doped carbon nanocomposites with tunable morphology: Synergistic ultrafast low-temperature synthesis and tetracycline adsorption. Sep. Purif. Technol., 2021, 278: 119548 doi: 10.1016/j.seppur.2021.119548
28. [28]
  Wang F, Zhang L J, Wang Y Y, Liu X J, Rohani S, Lu J. Fe₃O₄@ SiO₂@CS-TETA functionalized graphene oxide for the adsorption of methylene blue (MB) and Cu(Ⅱ). Appl. Surf. Sci., 2017, 420: 970-981 doi: 10.1016/j.apsusc.2017.05.179
29. [29]
  Zhou S, Xie Y X, Zhu F Y, Gao Y Y, Liu Y J, Tang Z P, Duan Y. Amidoxime modified chitosan/graphene oxide composite for efficient adsorption of U(Ⅵ) from aqueous solutions. J. Environ. Chem. Eng., 2021, 9(6): 106363 doi: 10.1016/j.jece.2021.106363
30. [30]
  Lin J Y, Liu Y, Hu S, Zhang Y F, Qian C, Li A M, Zhang S P. Ultra-fast adsorption of four typical pollutants using magnetically separable ethanolamine-functionalized graphene. Sep. Purif. Technol., 2021, 271: 118862 doi: 10.1016/j.seppur.2021.118862
31. [31]
  Liang L L, Gao S W, Zhu J C, Wang L J, Xiong Y N, Xia X F, Yang L W. The enhanced photocatalytic performance toward carbamazepine by nitrogen-doped carbon dots decorated on BiOBr/CeO₂: Mechanism insight and degradation pathways. Chem. Eng. J., 2020, 391: 123599 doi: 10.1016/j.cej.2019.123599
32. [32]
  Hailili R, Wang Z Q, Li Y X, Wang Y H, Sharma V, Gong X, Wang C Y. Oxygen vacancies induced visible-light photocatalytic activities of CaCu₃Ti₄O₁₂ with controllable morphologies for antibiotic degradation. Appl. Catal. B-Environ., 2018, 221: 422-432 doi: 10.1016/j.apcatb.2017.09.026
33. [33]
  Zhang Y, Zhou J B, Chen J H, Feng X Q, Cai W Q. Rapid degradation of tetracycline hydrochloride by heterogeneous photocatalysis coupling persulfate oxidation with MIL-53(Fe) under visible light irradiation. J. Hazard. Mater., 2020, 392: 122315-122326 doi: 10.1016/j.jhazmat.2020.122315
34. [34]
  Wang Y J, Qiu L Y, Bao S Y, Tian F, Sheng J, Yang W W, Yu Y S. Visible-light enhanced peroxymonosulfate activation on Co₃O₄/MnO₂ for the degradation of tetracycline: Cooperation of radical and non-radical mechanisms. Sep. Purif. Technol., 2023, 316: 123779 doi: 10.1016/j.seppur.2023.123779
35. [35]
  Jin L H, Amaya-Mazo X, Apel M, Sankisa S, Johnson E, Zbyszynska M, Han A. Ca²⁺ and Mg²⁺ bind tetracycline with distinct stoichiometries and linked deprotonation. Biophys. Chem., 2007, 128(2): 185-196
36. [36]
  Yang Y Y, Zhang X G, Niu C G, Feng H P, Qin P Z, Guo H, Liang C, Zhang L, Liu H Y, Li L. Dual-channel charges transfer strategy with synergistic effect of Z-scheme heterojunction and LSPR effect for enhanced quasi-full-spectrum photocatalytic bacterial inactivation: New insight into interfacial charge transfer and molecular oxygen activation. Appl. Catal. B-Environ., 2020, 264: 188465
37. [37]
  Yang Y J, Bian Z Y, Zhang L, Wang H. Bi@BiO_x(OH)_y modified oxidized g-C₃N₄ photocatalytic removal of tetracycline hydrochloride with highly effective oxygen activation. J. Hazard. Mater., 2022, 427: 127866 doi: 10.1016/j.jhazmat.2021.127866
38. [38]
  Zhang Q Z, Sun Y Q, Xu W J, Cao Y, Wu C F, Wang C, Tsang D. Efficient microwave-assisted mineralization of oxytetracycline driven by persulfate and hypochlorite over Cu-biochar catalyst. Bioresour. Technol., 2023, 372: 128698 doi: 10.1016/j.biortech.2023.128698
39. [39]
  Dias I, Mourão L, Andrade L, Souza G, Viana J, Oliveira S, Alonso C. Degradation of antibiotic amoxicillin from pharmaceutical industry wastewater into a continuous flow reactor using supercritical water gasification. Water Res., 2023, 234: 119826 doi: 10.1016/j.watres.2023.119826
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