Abstract
Layered double hydroxide (LDH) is an applicable material that can be modified in various ways. Modifications using natural extracts fulfill the principles of “green chemistry.” The preparation of butterfly pea flower extract (BPE)-modified NiAl LDH was completed using the calcination and restacking method. The characteristics of the prepared composites were identified through analysis of functional groups, crystal phase, bandgap energy, surface area and surface morphology. Fourier transform-infrared (FT-IR) characterization revealed that the active group of the catalyst is -OH except for NiAl layered double oxide (LDO), which has the metal oxide-like functional groups. X-ray diffraction patterns expressed a typical layered material structure of NiAl LDH dan NiAl LDH-BPE, but not for NiAl LDO and NiAl LDO-BPE. Introducing BPE into NiAl LDH and NiAl LDO effectively decreased the bandgap energy and changed the surface morphology. The prepared catalysts were applied in a batch system with pH 5 to degrade tetracycline (TC). NiAl LDO demonstrated the highest activity as a catalyst in TC degradation, with a 93.61% degradation rate. In contrast, NiAl LDO-BPE demonstrated the highest structural stability in TC degradation and repeated use, with an initial degradation percentage of 82.58% and a fifth regeneration percentage of 71.4%.
Similar content being viewed by others
References
Ahmad N, Arsyad FS, Royani I, Siregar PMSBN, Taher T, Lesbani A (2023a) High regeneration of ZnAl/NiAl-magnetite humic acid for adsorption of Congo red from aqueous solution. Inorg Chem Commun 150:110517. https://doi.org/10.1016/j.inoche.2023.110517
Ahmad N, Wibiyan S, Royani I, Mohadi R, Lesbani A (2023b) Reusable heterogeneous catalyst (M2+) Al-layered double hydroxide used for oxidative desulfurization of 4,6-dimethyldibenzothiophene. Indonesian J Mater Res 1(3):2–8
Amiri M, Salavati-Niasari M, Akbari A, Gholami T (2017) Removal of malachite green (a toxic dye) from water by cobalt ferrite silica magnetic nanocomposite: herbal and green sol-gel autocombustion synthesis. Int J Hydrogen Energy 42(39):24846–24860. https://doi.org/10.1016/j.ijhydene.2017.08.077
Angel Ezhilarasi A, Judith Vijaya J, Kaviyarasu K, John Kennedy L, Ramalingam RJ, Al-Lohedan HA (2018) Green synthesis of NiO nanoparticles using Aegle marmelos leaf extract for the evaluation of in-vitro cytotoxicity, antibacterial and photocatalytic properties. J Photochem Photobiol B 180:39–50. https://doi.org/10.1016/j.jphotobiol.2018.01.023
Azalok KA, Oladipo AA, Gazi M (2021) Hybrid MnFe-LDO–biochar nanopowders for degradation of metronidazole via UV-light-driven photocatalysis: Characterization and mechanism studies. Chemosphere 268:128844. https://doi.org/10.1016/j.chemosphere.2020.128844
Badri AF, Juleanti N, Palapa NR, Hanifah Y, Mohadi R, Mardiyanto, Lesbani A (2021) Oxalate intercalated Mg/Cr layered double hydroxide as adsorbent of methyl red and methyl orange from aqueous solution. Ecol Eng Environ Technol 22(3):71–81. https://doi.org/10.12912/27197050/135509
Bai L, Li Y, Fu J, Wang X, Zhang J, Lu J (2023) Purpurin intercalated layered double hydroxide nanocomposites for improved CO2 visible photocatalytic reduction: dye-intercalation stabilization and sensitization. Appl Surf Sci 639. https://doi.org/10.1016/j.apsusc.2023.158247
Beigi, F., Reza, A., Hossein, A., & Khavar, C. (2023). Applied surface science design and synthesis of Bi-doped NiAl-LDH / g-C3N4 heterostructure; a novel 2D / 2D system for simultaneous enhanced photocatalytic degradation and fluorescence sensing of ciprofloxacin. Appl Surf Sci, 637, 157972. https://doi.org/10.1016/j.apsusc.2023.157972
Chen P, Zhang Q, Zheng X, Tan C, Zhuo M, Chen T, Wang F, Liu H, Liu Y, Feng Y, Lv W, Liu G (2020) Phosphate-modified m-Bi2O4 enhances the absorption and photocatalytic activities of sulfonamide: mechanism, reactive species, and reactive sites. J Hazard Mater 384:121443. https://doi.org/10.1016/j.jhazmat.2019.121443
Chen Q, Wu L, Zhao X, Yang X (2022) Fabrication of Zn-Ti layered double oxide nanosheets with ZnO / ZnTiO3 heterojunction for enhanced photocatalytic degradation of MO, RhB and MB. J Mol Liq 353:118794. https://doi.org/10.1016/j.molliq.2022.118794
Deng J, Xiao L, Yuan S, Wang W, Zhan X, Hu Z (2021) Activation of peroxymonosulfate by CoFeNi layered double hydroxide / graphene oxide (LDH / GO) for the degradation of gatifloxacin. Sep Purif Technol 255:117685. https://doi.org/10.1016/j.seppur.2020.117685
Dharman RK, Shejale KP, Kim SY (2022) Efficient sonocatalytic degradation of heavy metal and organic pollutants using CuS/MoS2 nanocomposites. Chemosphere 305:135415. https://doi.org/10.1016/j.chemosphere.2022.135415
Ebrahimi M, Akhavan O (2022) Nanomaterials for photocatalytic degradations of analgesic, mucolytic and anti-biotic/viral/inflammatory drugs widely used in controlling SARS-CoV-2. Catalysts 12(6). https://doi.org/10.3390/catal12060667
Faisal S, Jan H, Shah SA, Shah S, Khan A, Akbar MT, Rizwan M, Jan F, Wajidullah, Akhtar N, Khattak A, Syed S (2021) Green synthesis of zinc oxide (ZnO) nanoparticles using aqueous fruit extracts of Myristica fragrans: their characterizations and biological and environmental applications. ACS Omega 6(14):9709–9722. https://doi.org/10.1021/acsomega.1c00310
Fatimah I, Sahroni I, Muraza O, Doong R (2020) Journal of Environmental Chemical Engineering One-pot biosynthesis of SnO2 quantum dots mediated by Clitoria ternatea flower extract for photocatalytic degradation of rhodamine B. J Environ Chem Eng 8(4):103879. https://doi.org/10.1016/j.jece.2020.103879
Gandamalla A, Manchala S, Verma A, Fu YP, Shanker V (2021) Microwave-assisted synthesis of ZnAl-LDH/g-C3N4 composite for degradation of antibiotic ciprofloxacin under visible-light illumination. Chemosphere 283:131182. https://doi.org/10.1016/j.chemosphere.2021.131182
Gholami P, Khataee A, Soltani RDC, Dinpazhoh L, Bhatnagar A (2020) Photocatalytic degradation of gemifloxacin antibiotic using Zn-Co-LDH@biochar nanocomposite. J Hazard Mater 382:121070. https://doi.org/10.1016/j.jhazmat.2019.121070
Huang W, Li Y, Fu Q, Chen M (2022) Fabrication of a novel biochar decorated nano-flower-like MoS2 nanomaterial for the enhanced photodegradation activity of ciprofloxacin: Performance and mechanism. Mater Res Bull 147:111650. https://doi.org/10.1016/j.materresbull.2021.111650
Isnaeni IN, Indriyati, Dedi, Sumiarsa D, Primadona I (2021) Green synthesis of different TiO2 nanoparticle phases using mango-peel extract. Mater Lett 294:129792. https://doi.org/10.1016/j.matlet.2021.129792
Kameda T, Ikeda D, Kumagai S, Saito Y, Yoshioka T (2020) Adsorption of SeO42− by delaminated Mg-Al layered double hydroxide nanosheets. Inorg Chem Commun 122:108266. https://doi.org/10.1016/j.inoche.2020.108266
Khojasteh H, Salavati-Niasari M, Safajou H, Safardoust-Hojaghan H (2017) Facile reduction of graphene using urea in solid phase and surface modification by N-doped graphene quantum dots for adsorption of organic dyes. Diamond Relat Mater 79:133–144. https://doi.org/10.1016/j.diamond.2017.09.011
Kumar S, Isaacs MA, Trofimovaite R, Durndell L, Parlett CMA, Douthwaite RE, Coulson B, Cockett MCR, Wilson K, Lee AF (2017) P25@CoAl layered double hydroxide heterojunction nanocomposites for CO2 photocatalytic reduction. Appl Catal B Environ 209:394–404. https://doi.org/10.1016/j.apcatb.2017.03.006
Lesbani A, Taher T, Palapa NR, Mohadi R, Mardiyanto, Miksusanti, Arsyad FS (2021) Removal of malachite green dye using keggin polyoxometalate intercalated ZnAl layered double hydroxide. Walailak J Sci Technol 18(10):1–13. https://doi.org/10.48048/wjst.2021.9414
Lesbani A, Taher T, Palapa NR, Mohadi R, Rachmat A, Mardiyanto. (2020) Preparation and utilization of Keggin-type polyoxometalate intercalated Ni–Fe layered double hydroxides for enhanced adsorptive removal of cationic dye. SN Appl Sci 2(3):4–7. https://doi.org/10.1007/s42452-020-2300-8
Li T, Miras HN, Song YF (2017) Polyoxometalate (POM)-Layered Double Hydroxides (LDH) composite materials: design and catalytic applications. Catalysts 7(9):7–10. https://doi.org/10.3390/catal7090260
Li Z, Li H, Zeng X, Liu S, Yang Y (2023) Adsorption and photodegradation of tetracycline by mannose-grafted chitosan composite films: performance, mechanism and availability. Chem Eng J 458. https://doi.org/10.1016/j.cej.2023.141455
Lu Y, Ding C, Guo J, Gan W, Chen P, Zhang M, Sun Z (2022) Highly efficient photodegradation of ciprofloxacin by dual Z-scheme Bi2MoO6/GQDs/TiO2 heterojunction photocatalysts: mechanism analysis and pathway exploration. J Alloys Compd 924:166533. https://doi.org/10.1016/j.jallcom.2022.166533
Ma Q, Han X, Cui J, Zhang Y, He W (2022) Ni embedded carbon nanofibers/ Ni-Al LDHs with multicomponent synergy for hybrid supercapacitor electrodes. Colloids Surf A Physicochem Eng Asp 649:129270. https://doi.org/10.1016/j.colsurfa.2022.129270
Mir N, Salavati-Niasari M (2013) Preparation of TiO2 nanoparticles by using tripodal tetraamine ligands as complexing agent via two-step sol–gel method and their application in dye-sensitized solar cells. Mater Res Bull 48(4):1660–1667. https://doi.org/10.1016/j.materresbull.2013.01.006
Muhire C, Zhang D, Xu X (2022) Adsorption of uranium (VI) ions by LDH intercalated with L-methionine in acidic water: kinetics, thermodynamics and mechanisms. Results Eng 16:100686. https://doi.org/10.1016/j.rineng.2022.100686
Muráth S, Dvorníková N, Moreno-Rodríguez D, Novotný R, Pospíšil M, Urbanová M, Brus J, Kovanda F (2023) Intercalation of atorvastatin and valsartan into Mg Al layered double hydroxide host using a restacking procedure. Appl Clay Sci 231:106717. https://doi.org/10.1016/j.clay.2022.106717
Ni J, Jing B, Lin J, Lin B, Zhao Z, Jiang L (2018) Effect of rare earth on the performance of Ru/MgAl-LDO catalysts for ammonia synthesis. J Rare Earths 36(2):135–141. https://doi.org/10.1016/j.jre.2017.07.011
Oladipo AA (2021) Journal of water process engineering rapid photocatalytic treatment of high-strength olive mill wastewater by sunlight and UV-induced CuCr2O4@CaFe–LDO. J Water Process Eng 40:101932. https://doi.org/10.1016/j.jwpe.2021.101932
Palapa NR, Taher T, Mohadi R, Rachmat A, Mardiyanto M, Miksusanti M, Lesbani A (2022) NiAl-layered double hydroxide intercalated with Keggin polyoxometalate as adsorbent of malachite green: kinetic and equilibrium studies. Chem Eng Commun 209(5):684–695. https://doi.org/10.1080/00986445.2021.1895773
Palapa NR, Wijaya A (2023) Layered double hydroxide coated by carbon-based material for environmental dye pollutant. 1(3). https://doi.org/10.26554/ijmr.20231311
Panahi-Kalamuei M, Salavati-Niasari M, Hosseinpour-Mashkani SM (2014) Facile microwave synthesis, characterization, and solar cell application of selenium nanoparticles. J Alloys Compd 617:627–632. https://doi.org/10.1016/j.jallcom.2014.07.174
Prabhu S, Daniel Thangadurai T, Vijai Bharathy P, Kalugasalam P (2022a) Synthesis and characterization of nickel oxide nanoparticles using Clitoria ternatea flower extract: photocatalytic dye degradation under sunlight and antibacterial activity applications. Results Chem 4:100285. https://doi.org/10.1016/j.rechem.2022.100285
Prabhu S, Thangadurai TD, Indumathi T, Kalugasalam P (2022b) Enhanced visible light induced dye degradation and antibacterial activities of ZnO / NiO nanocomposite synthesized using Clitoria ternatea flower extract. Inorg Chem Commun 146:110077. https://doi.org/10.1016/j.inoche.2022.110077
Priya P, Elumali K, Shakila D, Geetha K, Karthik AD (2020) Materials today: proceedings facile approach to synthesize , compared to MgO & ZnO nanoparticles by using Clitoria ternatea / Tecoma castanifolia flower. Mater Today Proc 29:1217–1222. https://doi.org/10.1016/j.matpr.2020.05.479
Priyadharsan A, Vasanthakumar V, Karthikeyan S, Raj V, Shanavas S, Anbarasan PM (2017) Multi-functional properties of ternary CeO2/SnO2/rGO nanocomposites: visible light driven photocatalyst and heavy metal removal. J Photochem Photobiol A Chem 346:32–45. https://doi.org/10.1016/j.jphotochem.2017.05.030
Ran Z, Shao X, Mushtaq MA, Du X, Liu H, Hou S, Ji S (2022) Preparation of Cs/Cu-LDO@X catalysts and reaction mechanism of the side-chain alkylation of toluene to styrene. Catal Today 402:122–137. https://doi.org/10.1016/j.cattod.2022.03.026
Rohmatullaili, Ahmad, N., Erviana, D., Savira, D., Mohadi, R., & Lesbani, A. (2024a). ZnAl LDH-based derivative materials as photocatalysts: synthesis, characterization, and catalytic performance in tetracycline degradation. Sci Technol Indonesia, 9(2). https://doi.org/10.26554/sti.2024.9.2.457-469 1.
Rohmatullaili, Ahmad N, Savira D, Erviana D, Zultriana, Mohadi R, Lesbani A (2024b) A series of MgAl layer double hydroxide-based materials intercalated with Clitoria ternatea flower extract as photocatalysts in the ciprofloxacin degradation. Chem Phys Impact 8:100587. https://doi.org/10.1016/j.chphi.2024.100587
Rohmatullaili R, Ahmad N, Erviana D, Zultriana Z, Savira D, Mohadi R, Lesbani A (2024c) Enhancing the performance of modified ZnAl LDH as hybrid catalyst- adsorbent on tetracycline removal under solar light irradiation. Inorg Chem Commun:112101. https://doi.org/10.1016/j.inoche.2024.112101
Romero Ortiz G, Lartundo-Rojas L, Samaniego-Benítez JE, Jiménez-Flores Y, Calderón HA, Mantilla A (2021) Photocatalytic behavior for the phenol degradation of ZnAl layered double hydroxide functionalized with SDS. J Environ Manage 277:1–8. https://doi.org/10.1016/j.jenvman.2020.111399
Salavati-Niasari M, Dadkhah M, Davar F (2009) Pure cubic ZrO2 nanoparticles by thermolysis of a new precursor. Polyhedron 28(14):3005–3009. https://doi.org/10.1016/j.poly.2009.06.032
Shakeri B, Heidari E, Boutorabi SMA (2023) Effect of isothermal heat treatment time on the microstructure and properties of 4.3% Al austempered ductile iron. Int J Met 17(4):3005–3018. https://doi.org/10.1007/s40962-023-00980-4
Shen JC, Zeng HY, Chen CR, Xu S (2020) A facile fabrication of Ag2O-Ag/ZnAl-oxides with enhanced visible-light photocatalytic performance for tetracycline degradation. Appl Clay Sci 185:105413. https://doi.org/10.1016/j.clay.2019.105413
Silaen L, Palapa NR, Elfita, Mohadi R, Lesbani A (2021) Intercalated zn-cr-[α-siw12o40] as removal agents of cobalt (Ii) in watery phase: adsorption and regeneration study. Chiang Mai J Sci 48(2):545–556
Silva-Osuna ER, Vilchis-Nestor AR, Villarreal-Sanchez RC, Castro-Beltran A, Luque PA (2022) Study of the optical properties of TiO2 semiconductor nanoparticles synthesized using Salvia rosmarinus and its effect on photocatalytic activity. Opt Mater 124:112039. https://doi.org/10.1016/j.optmat.2022.112039
Siregar PMSBN, Palapa NR, Wijaya A, Fitri ES, Lesbani A (2021) Structural stability of ni/al layered double hydroxide supported on graphite and biochar toward adsorption of congo red. Sci Technol Indonesia 6(2):85–95. https://doi.org/10.26554/STI.2021.6.2.85-95
Teymourinia H, Salavati-Niasari M, Amiri O, Safardoust-Hojaghan H (2017) Synthesis of graphene quantum dots from corn powder and their application in reduce charge recombination and increase free charge carriers. J Mol Liq 242:447–455. https://doi.org/10.1016/j.molliq.2017.07.052
Thi N, Huyen K, Pham T, Thi N, Cam D (2021) Fabrication of titanium doped BiVO4 as a novel visible light driven photocatalyst for degradation of residual tetracycline pollutant. Ceram Int 47(24):34253–34259. https://doi.org/10.1016/j.ceramint.2021.08.335
Villegas-Fuentes A, Garrafa-Gálvez HE, Quevedo-Robles RV, Luque-Morales M, Vilchis-Nestor AR, Luque PA (2023) Synthesis of semiconductor ZnO nanoparticles using Citrus microcarpa extract and the influence of concentration on their optical properties. J Mol Struct 1281. https://doi.org/10.1016/j.molstruc.2023.135067
Wang B, Wei S, Wang Y, Huang W, Liang Y, Guo L, Xue J, Lu F, Liu Z, Xu B (2023) Colloids and surfaces A: physicochemical and engineering aspects high energy ball-milled nano-Ti polymer: kinetic analysis and synergetic effect. Colloids Surf A Physicochem Eng Asp 656(PA):130305. https://doi.org/10.1016/j.colsurfa.2022.130305
Wang Y, Liu T, Xie Y, Li N, Liu Y, Wen J, Zhang M, Feng W, Huang J, Guo Y, Kabbas T, Wang D, Granato D (2022) Clitoria ternatea blue petal extract protects against obesity, oxidative stress, and inflammation induced by a high-fat, high-fructose diet in C57BL/6 mice. Food Res Int 162. https://doi.org/10.1016/j.foodres.2022.112008
Yao Y, Yu F, Li J, Li J, Li Y, Wang Z, Zhu M (2019) Two-dimensional NiAl layered double oxides as non-noble metal catalysts for enhanced CO methanation performance at low temperature. Fuel 255:115770. https://doi.org/10.1016/j.fuel.2019.115770
Ye H, Liu S, Yu D, Zhou X, Qin L, Lai C, Qin F, Zhang M, Chen W, Chen W, Xiang L (2022) Regeneration mechanism, modification strategy, and environment application of layered double hydroxides: Insights based on memory effect. Coord Chem Rev 450:214253. https://doi.org/10.1016/j.ccr.2021.214253
Yuliasari N, Amri, Mohadi R, Elfita, Lesbani A (2022) Improvement of Congo Red photodegradation performance through Zn/Al-TiO2 and Zn/Al-ZnO preparation. Sci Technol Indonesia 7(4):449–454. https://doi.org/10.26554/sti.2022.7.4.449-454
Zhang C, Wang J, Liu Y, Lin L, Lei L, Zhang H, Wang Z, Cheng H, Wang P, Zheng Z, Huang B (2022) Enhanced photocatalytic driven hydroxylation of phenylboric acid to phenol over pyrenetetrasulfonic acid intercalated ZnAl-LDHs. J Colloid Interface Sci 610:455–462. https://doi.org/10.1016/j.jcis.2021.12.005
Acknowledgements
The authors thank the Research Center of Inorganic Materials and Complexes Universitas Sriwijaya for the chemicals, laboratory equipment, and characterization. The authors also thank the Integrated Laboratory of UIN Raden Fatah Palembang for instrumental analysis.
Author information
Authors and Affiliations
Contributions
R.R.: writing-original draft, conceptualization, investigation, writing-review and editing
N.A.: writing-review and editing, software
Z.Z.: investigation, formal analysis, visualization
D.S.: investigation, visualization, data curation
D.E.: formal analysis, validation, software
R.M.: methodology, validation, software
A.L.: conceptualization, methodology, writing-review and editing, supervision
Corresponding author
Ethics declarations
Ethical approval
Hereby, the author consciously ensures that the manuscript “High Stability and Selectivity of Butterfly Pea Flower Extract-NiAl LDH-based Catalysts in the Tetracycline Degradation” fulfills the following matters:
-
1)
This paper is the author’s own original work, which has not been previously published elsewhere.
-
2)
This paper is not currently being considered for publication elsewhere.
-
3)
This paper reflects the author’s own research and analysis honestly and completely.
-
4)
This paper gives due recognition to the significant contributions of co-authors and fellow researchers.
-
5)
The results are appropriately placed in the context of previous and existing research.
-
6)
All sources used are disclosed correctly (correct citations). Literal copying of text should be indicated by using quotation marks and providing appropriate references.
-
7)
All authors have been personally and actively involved in the important work leading to this paper and will take public responsibility for its contents.
I agree with the above statement and declare that this submission follows Springer policies as outlined in the Guidelines for Authors and Ethical Statement.
Consent to participate
Informed consent was obtained from all individual participants. included in the study.
Consent for publication
The authors have agreed to submit the results of this study for publication.
Competing interests
The authors declare no competing interests.
Additional information
Responsible Editor: George Z. Kyzas
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Rohmatullaili, R., Ahmad, N., Zultriana, Z. et al. High stability and selectivity of butterfly pea flower extract-NiAl LDH-based catalysts in the tetracycline degradation. Environ Sci Pollut Res 31, 33107–33119 (2024). https://doi.org/10.1007/s11356-024-33445-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-024-33445-0