Skip to main content
Log in

A co-precipitation route for the preparation of eco-friendly Cu-Al-layered double hydroxides with efficient tetracycline degradation

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

The construction of novel efficient catalysts for the treatment of organic pollutants in the aqueous environment is essential. The lamellar-like Cu-Al layered double hydroxides (CuAl-LDHs) with various mole ratios were synthesized by a simple route of co-precipitation, and the corresponding degradation characteristic was tested for the removal of tetracycline (TC) using PMS activation. The degradation efficiency of TC over CuAl-LDHs increased up to 93% within 10 min for the Cu/Al mole ratio of 3:1 and almost not changed at a higher mole ratio. For further calcining the optimal catalyst at 300 ℃, the degradation efficiency of TC was found to be increased to 96%. Sulfuric radicals and singlet oxygen were analyzed to be the main reason for the change in degradation characteristics, which was proved by radical quenching experiments and electron paramagnetic resonance technique. The parameters including PMS concentration, catalyst dosage, and reaction temperature on the TC degradation as well as the degradation mechanism for PMS activation were elaborated. The best proportion of CuAl-LDHs owned splendid stability and catalytic activity after reusing, which showed enormous potential in practical application.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11
Fig. 12
Fig. 13
Fig. 14
Fig. 15

Similar content being viewed by others

Data availability

Data and materials are available upon reasonable request.

References

  • Abazari R, Mahjoub AR, Sanati S, Rezvani Z, Hou ZQ, Dai HX (2019) Ni-Ti layered double hydroxide@graphitic carbon nitride nanosheet: a novel nanocomposite with high and ultrafast sonophotocatalytic performance for degradation of antibiotics. Inorg Chem 58:1834–1849

    CAS  Google Scholar 

  • Bezryadina Anna S, Preece Daryl C, Chen Joseph C, Chen Z (2016) Optical disassembly of cellular clusters by tunable tug-of-war tweezers. Light-Sci Appl 5:1–8

    Google Scholar 

  • Bharali D, Deka RC (2017) Preferential adsorption of various anionic and cationic dyes from aqueous solution over ternary CuMgAl layered double hydroxide. Colloid Surf A-Physicochem Eng Asp 525:64–76

    CAS  Google Scholar 

  • Bridier B, Lopez N, Perez-Ramirez J (2010) Partial hydrogenation of propyne over copper-based catalysts and comparison with nickel-based analogues. J Catal 269:80–92

    CAS  Google Scholar 

  • Bukhtiyarova MV (2019) A review on effect of synthesis conditions on the formation of layered double hydroxides. J Solid State Chem 269:494–506

    CAS  Google Scholar 

  • Cao J, Sun SW, Li X, Yang ZH, Xiong WP, Wu Y, Jia MY, Zhou YY, Zhou CY, Zhang YR (2020) Efficient charge transfer in aluminum-cobalt layered double hydroxide derived from Co-ZIF for enhanced catalytic degradation of tetracycline through peroxymonosulfate activation. Chem Eng J 382:122802

    CAS  Google Scholar 

  • Chakraborty A, Islam DA, Acharya H (2019) One pot synthesis of ZnO-CuO nanocomposites for catalytic peroxidase like activity and dye degradation. Mater Res Bull 120:110592

    CAS  Google Scholar 

  • Chen MQ, Wu PX, Huang ZY, Liu JQ, Li YH, Zhu NW, Dang Z, Bi YZ (2019) Environmental application of MgMn-layered double oxide for simultaneous efficient removal of tetracycline and Cd pollution: performance and mechanism. J Environ Manag 246:164–173

    CAS  Google Scholar 

  • Chen GY, Sun YB, Shi PC, Liu T, Li ZH, Luo SH, Wang XC, Cao XY, Ren B, Liu GK, Yang LL, Tian ZQ (2021) Revealing unconventional host-guest complexation at nanostructured interface by surface-enhanced Raman spectroscopy. Light-Sci Appl 10:85–93

    CAS  Google Scholar 

  • Cosano D, Esquivel D, Romero FJ, Jimenez-Sanchidrian C, Ruiz JR (2019) Microwave-assisted synthesis of hybrid organo-layered double hydroxides containing cholate and deoxycholate. Mater Chem Phys 225:28–33

    CAS  Google Scholar 

  • Cunha VRR, Petersen PAD, Goncalves MB, Petrilli HM, Taviot-Gueho C, Leroux F, Temperini MLA, Constantino VRL (2012) Structural, spectroscopic (NMR, IR, and Raman), and DFT investigation of the self-assembled nanostructure of pravastatin-LDH (layered double hydroxides) systems. Chem Mat 24:1415–1425

    CAS  Google Scholar 

  • de Matos CS, Nobrega MM, Temperini MLA, Constantino VRL (2019) Hybrid Ni-Al layered double hydroxide: characterization and in situ synchrotron XRD and vibrational spectroscopic studies under high-pressure. Appl Clay Sci 174:152–158

    Google Scholar 

  • Dong YN, Hu TD, Pudukudy M, Su HY, Jiang LH, Shan SY, Jia QM (2020) Influence of microwave-assisted synthesis on the structural and textural properties of mesoporous MIL-101(Fe) and NH2-MIL-101(Fe) for enhanced tetracycline adsorption. Mater Chem Phys 251:123060

    CAS  Google Scholar 

  • Fu XM, Ren XQ, Shen JC, Jiang Y, Wang YH, Orooji Y, Xu WL, Liang JH (2021) Synergistic catalytic hydrogenation of furfural to 1,2-pentanediol and 1,5-pentanediol with LDO derived from CuMgAl hydrotalcite. Mol Catal 499:111298

    CAS  Google Scholar 

  • Ghanbari F, Moradi M (2017) Application of peroxymonosulfate and its activation methods for degradation of environmental organic pollutants: Review. Chem Eng J 310:41–62

    CAS  Google Scholar 

  • Gong C, Chen F, Yang Q, Luo K, Yao FB, Wang SN, Wang XL, Wu JW, Li XM, Wang DB, Zeng GM (2017) Heterogeneous activation of peroxymonosulfate by Fe-Co layered doubled hydroxide for efficient catalytic degradation of Rhoadmine B. Chem Eng J 321:222–232

    CAS  Google Scholar 

  • Hassani A, Eghbali P, Mahdipour F, Waclawek S, Lin KYA, Ghanbari F (2023a) Insights into the synergistic role of photocatalytic activation of peroxymonosulfate by UVA-LED irradiation over CoFe2O4-rGO nanocomposite towards effective bisphenol A degradation: performance, mineralization, and activation mechanism. Chem Eng J 453:139556

    CAS  Google Scholar 

  • Hassani A, Scaria J, Ghanbari F, Nidheesh PV (2023b) Sulfate radicals-based advanced oxidation processes for the degradation of pharmaceuticals and personal care products: a review on relevant activation mechanisms, performance, and perspectives. Environ Res 217:114789

    CAS  Google Scholar 

  • He Y, Wang R, Jiao TF, Yan XY, Wang ML, Zhang LX, Bai ZH, Zhang Q, Peng QM (2019) Facile preparation of self-assembled layered double hydroxide-based composite dye films as new chemical gas sensors. ACS Sustain Chem Eng 7:10888–10899

    CAS  Google Scholar 

  • Hong YC, Peng JL, Zhao XG, Yan Y, Lai B, Yao G (2019) Efficient degradation of atrazine by CoMgAl layered double oxides catalyzed peroxymonosulfate: optimization, degradation pathways and mechanism. Chem Eng J 370:354–363

    CAS  Google Scholar 

  • Hou LH, Li XM, Yang Q, Chen F, Wang SN, Ma YH, Wu Y, Zhu XF, Huang XD, Wang DB (2019) Heterogeneous activation of peroxymonosulfate using Mn-Fe layered double hydroxide: performance and mechanism for organic pollutant degradation. Sci Total Environ 663:453–464

    CAS  Google Scholar 

  • Hu SF, Sun Y, Pu M, Yun RP, Xiang X (2019) Determination of boundary conditions for highly efficient separation of magnesium and lithium from salt lake brine by reaction-coupled separation technology. Sep Purif Technol 229:115813

    CAS  Google Scholar 

  • Jia Z, Wang JC, Liang SX, Zhang WC, Wang WM, Zhang LC (2017) Activation of peroxymonosulfate by Fe78Si9B13 metallic glass: the influence of crystallization. J Alloy Compd 728:525–533

    CAS  Google Scholar 

  • Karim AV, Hassani A, Eghbali P, Nidheesh PV (2022) Nanostructured modified layered double hydroxides (LDHs)-based catalysts: a review on synthesis, characterization, and applications in water remediation by advanced oxidation processes. Curr Opin Solid State Mat Sci 26:100965

    CAS  Google Scholar 

  • Kaur P, Singh S, Deepeka BV, Kumar V, Tikoo KB, Kaushik A, Singhal S (2021) Aggrandized catalytic performance of transition metal doped strontium hexagonal ferrites for the treatment of malevolent organic pollutants. J Alloy Compd 856:158026

    CAS  Google Scholar 

  • Kim W, Mohaideen KK, Seo DJ, Yoon WL (2017) Methanol-steam reforming reaction over Cu-Al-based catalysts derived from layered double hydroxides. Int J Hydrog Energy 42:2081–2087

    CAS  Google Scholar 

  • Kuld S, Conradsen C, Moses PG, Chorkendorff I, Sehested J (2014) Quantification of zinc atoms in a surface alloy on copper in an industrial-type methanol synthesis catalyst. Angew Chem-Int Edit 53:5941–5945

    CAS  Google Scholar 

  • Li S, Shi WZ, Liu W, Li HM, Zhang W, Hu JR, Ke YC, Sun WL, Ni JR (2018) A duodecennial national synthesis of antibiotics in China’s major rivers and seas (2005–2016). Sci Total Environ 615:906–917

    CAS  Google Scholar 

  • Li DY, Fan LH, Shen YM, Qi M, Ali MDR, Liu DB, Li SF (2019a) Degradation of rhodamine B under visible-light by Cu-doped ZnAl layered double hydroxide. J Nanosci Nanotechnol 19:1090–1097

    Google Scholar 

  • Li LQ, Zhao JH, Xiao YY, Huang ZQ, Guo ZZ, Li FX, Deng LQ (2019b) Flotation performance and adsorption mechanism of malachite with tert-butylsalicylaldoxime. Sep Purif Technol 210:843–849

    CAS  Google Scholar 

  • Li XM, Yan XL, Hu XY, Feng R, Zhou M, Wang LP (2020) Hollow Cu-Co/N-doped carbon spheres derived from ZIFs as an e fficient catalyst for peroxymonosulfate activation. Chem Eng J 397:125533

    CAS  Google Scholar 

  • Liao ZW, Dai SJ, Long SJ, Yu YJ, Ali J, Wang HB, Chen ZL, Chen ZQ (2018) Pd based in situ AOPs with heterogeneous catalyst of FeMgAl layered double hydrotalcite for the degradation of bisphenol A and landfill leachate through multiple pathways. Environ Sci Pollut Res 25:35623–35636

    CAS  Google Scholar 

  • Lin GH, Zhu L, Duan T, Zhang L, Liu B, Lei JH (2019) Efficient capture of iodine by a polysulfide-inserted inorganic NiTi-layered double hydroxides. Chem Eng J 378:122181

    CAS  Google Scholar 

  • Liu XH, Lu SY, Guo W, Xi BD, Wang WL (2018) Antibiotics in the aquatic environments: a review of lakes. China Sci Total Environ 627:1195–1208

    CAS  Google Scholar 

  • Liu S, Liu J, Liu GY, Liu YC, Zhong H (2020) Modulation of the morphology, surface energy and wettability of malachite through a S, O, O-ligand surfactant: Mechanism and hydrophobization. Appl Surf Sci 505:144467

    CAS  Google Scholar 

  • Lu HT, Sui MH, Yuan BJ, Wang JY, Lv YN (2019) Efficient degradation of nitrobenzene by Cu-Co-Fe-LDH catalyzed peroxymonosulfate to produce hydroxyl radicals. Chem Eng J 357:140–149

    CAS  Google Scholar 

  • Luo L, Wang YL, Zhu ML, Cheng XW, Zhang XL, Meng XZ, Huang X, Hao HX (2019) Co-Cu-Al layered double oxides as heterogeneous catalyst for enhanced degradation of organic pollutants in wastewater by activating peroxymonosulfate: performance and synergistic effect. Ind Eng Chem Res 58:8699–8711

    CAS  Google Scholar 

  • Luo YY, Liu C, Zhao MQ (2022) CoFe-LDO nanoparticles as a novel catalyst of peroxymonosulfate (PMS) for histidine removal. Environ Sci Pollut Res 29:16517–16528

    CAS  Google Scholar 

  • Lyu L, Yan DB, Yu GF, Cao WR, Hu C (2018) Efficient destruction of pollutants in water by a dual-reaction center fenton-like process over carbon nitride compounds-complexed Cu(II)-CuAlO2. Environ Sci Technol 52:4294–4304

    CAS  Google Scholar 

  • Ma JF, Ding JF, Li LY, Zou J, Kong Y, Komarneni S (2015) In situ reduction for synthesis of nano-sized Cu2O particles on MgCuAl-LDH layers for degradation of orange II under visible light. Ceram Int 41:3191–3196

    CAS  Google Scholar 

  • Ma XC, Dai Y, Yu L, Huang BB (2016) Energy transfer in plasmonic photocatalytic composites. Light-Sci Appl 5:e16017–e16030

    CAS  Google Scholar 

  • Madihi-Bidgoli S, Asadnezhad S, Yaghoot-Nezhad A, Hassani A (2021) Azurobine degradation using Fe2O3@multi-walled carbon nanotube activated peroxymonosulfate (PMS) under UVA-LED irradiation: performance, mechanism and environmental application. J Environ Chem Eng 9:106660

    CAS  Google Scholar 

  • Marques BS, Dalmagro K, Moreira KS, Oliveira MLS, Jahn SL, Burgo TAD, Dotto GL (2020) Ca -Al, Ni-Al and Zn-Al LDH powders as efficient materials to treat synthetic effluents containing o-nitrophenol. J Alloy Compd 838:155628

    CAS  Google Scholar 

  • Motlagh PY, Khataee A, Rad TS, Hassani A, Joo SW (2019) Fabrication of ZnFe-layered double hydroxides with graphene oxide for efficient visible light photocatalytic performance. J Taiwan Inst Chem Eng 101:186–203

    Google Scholar 

  • Oh WD, Dong ZL, Lim TT (2016) Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal: Current development, challenges and prospects. Appl Catal B-Environ 194:169–201

    CAS  Google Scholar 

  • Pi ZJ, Li XM, Wang DB, Xu QX, Tao ZLT, Huang XD, Yao FB, Wu Y, He L, Yang Q (2019) Persulfate activation by oxidation biochar supported magnetite particles for tetracycline removal: performance and degradation pathway. J Clean Prod 235:1103–1115

    CAS  Google Scholar 

  • Qiu Z, Tai CW, Niklasson GA, Edvinsson T (2019) Direct observation of active catalyst surface phases and the effect of dynamic self-optimization in NiFe-layered double hydroxides for alkaline water splitting. Energy Environ Sci 12:572–581

    CAS  Google Scholar 

  • Sun YX, Wang L, Wang T, Liu XQ, Xu T, Wei MB, Yang LL, Li CX (2021) Improved photocatalytic activity of Ni2P/NiCo-LDH composites via a Co-P bond charge transfer channel to degrade tetracycline under visible light. J Alloy Compd 862:158039

    CAS  Google Scholar 

  • Tian QZ, Sasaki K (2019) A novel composite of layered double hydroxide/geopolymer for co-immobilization of Cs+ and SeO42- from aqueous solution. Sci Total Environ 695:133799

    CAS  Google Scholar 

  • Tian WJ, Zhang HY, Qian Z, Ouyang TH, Sun HQ, Qin JY, Tade MO, Wang SB (2018) Bread-making synthesis of hierarchically Co@C nanoarchitecture in heteroatom doped porous carbons for oxidative degradation of emerging contaminants. Appl Catal B-Environ 225:76–83

    CAS  Google Scholar 

  • Tu D, Xu CN, Fujio Y, Yoshida A (2015) Mechanism of mechanical quenching and mechanoluminescence in phosphorescent CaZnOS:Cu. Light-Sci Appl 4:1–7

    Google Scholar 

  • Wang FF, Zhang YW, Liang WX, Chen LX, Li YJ, He XW (2018) Non-enzymatic glucose sensor with high sensitivity based on Cu-Al layered double hydroxides. Sens Actuator B-Chem 273:41–47

    CAS  Google Scholar 

  • Wong KT, Saravanan P, Nah IW, Choi J, Park C, Kim N, Yoon Y, Jang M (2019) Sonocatalytic reduction of nitrate using magnetic layered double hydroxide: Implications for removal mechanism. Chemosphere 218:799–809

    CAS  Google Scholar 

  • Yang S, Yao J, Quan Y, Hu M, Su R, Gao M, Han D, Yang J (2020) Monitoring the charge-transfer process in a Nd-doped semiconductor based on photoluminescence and SERS technology. Light-Sci Appl 9:117–124

    CAS  Google Scholar 

  • Yang HW, Zhou J, Yang EX, Li HX, Wu SJ, Yang W, Wang H (2021) Magnetic Fe3O4-N-doped carbon sphere composite for tetracycline degradation by enhancing catalytic activity for peroxymonosulfate: a dominant non-radical mechanism. Chemosphere 263:128011

    CAS  Google Scholar 

  • Yang JF, Li ZQ, Niu XR, Xu J, Shang N, Lei WX, Wu H (2022) Hierarchical porous N-doped carbon encapsulated CoFe2O4-CoO nanoparticles derived from layered double hydroxide/chitosan biocomposite for the enhanced degradation of tetracycline. Sep Purif Technol 295:121291

    CAS  Google Scholar 

  • Ye Q, Xu H, Zhang J, Wang QG, Zhou P, Wang YQ, Huang X, Huo XW, Liu CR, Lu JF (2020) Enhancement of peroxymonosulfate activation for antibiotics removal by nano zero valent tungsten induced Cu(II)/Cu(I) redox cycles. Chem Eng J 382:123054

    CAS  Google Scholar 

  • Yu XP, Zhang FB, Wang Y, Cheng DJ (2021) Easily recycled CuMgFe catalysts derived from layered double hydroxides for hydrogenolysis of glycerol. Catalysts 11:1–13

    Google Scholar 

  • Zeng HX, Zhang WQ, Deng L, Luo JM, Zhou SQ, Liu X, Pei Y, Shi Z, Crittenden J (2018) Degradation of dyes by peroxymonosulfate activated by ternary CoFeNi-layered double hydroxide: catalytic performance, mechanism and kinetic modeling. J Colloid Interface Sci 515:92–100

    CAS  Google Scholar 

  • Zeng HX, Deng L, Shi Z, Luo JM, Crittenden J (2019a) Heterogeneous degradation of carbamazepine by Prussian blue analogues in the interlayers of layered double hydroxides: performance, mechanism and toxicity evaluation. J Mater Chem A 7:342–352

    CAS  Google Scholar 

  • Zeng ZT, Ye SJ, Wu HP, Xiao R, Zeng GM, Liang J, Zhang C, Yu JF, Fang YL, Song B (2019b) Research on the sustainable efficacy of g-MoS2 decorated biochar nanocomposites for removing tetracycline hydrochloride from antibiotic-polluted aqueous solution. Sci Total Environ 648:206–217

    CAS  Google Scholar 

  • Zeng HX, Zhang HJ, Deng L, Shi Z (2020) Peroxymonosulfate-assisted photocatalytic degradation of sulfadiazine using self-assembled multi-layered CoAl-LDH/g-C3N4 heterostructures: performance, mechanism and eco-toxicity evaluation. J Water Process Eng 33:101084

    Google Scholar 

  • Zhang HJ, Li GC, Deng L, Zeng HX, Shi Z (2019a) Heterogeneous activation of hydrogen peroxide by cysteine intercalated layered double hydroxide for degradation of organic pollutants: performance and mechanism. J Colloid Interface Sci 543:183–191

    CAS  Google Scholar 

  • Zhang YY, Zhang LJ, Hu L, Huang SL, Jin ZY, Zhang M, Huang XY, Lu JG, Ruan SC, Zeng YJ (2019b) Multifunctional Zn-Al layered double hydroxides for surface-enhanced Raman scattering and surface-enhanced infrared absorption. Dalton Trans 48:426–434

    CAS  Google Scholar 

  • Zhang Z, Hua Z, Lang JH, Song YX, Zhang Q, Han Q, Fan HG, Gao M, Li XY, Yang JH (2019c) Eco-friendly nanostructured Zn-Al layered double hydroxide photocatalysts with enhanced photocatalytic activity. CrystEngComm 21:4607–4619

    CAS  Google Scholar 

  • Zhang P, He T, Chen H, Li P, Xiang MX, Ding NS, Deng SG (2020) The tetracyclines removal by MgAl layered double oxide in the presence of phosphate or nitrate: Behaviors and mechanism exploration. J Colloid Interface Sci 578:124–134

    CAS  Google Scholar 

  • Zhao XF, Niu CG, Zhang L, Guo H, Wen XJ, Liang C, Zeng GM (2018) Co-Mn layered double hydroxide as an effective heterogeneous catalyst for degradation of organic dyes by activation of peroxymonosulfate. Chemosphere 204:11–21

    CAS  Google Scholar 

  • Zhou L, Slany M, Bai BB, Du WC, Qu CT, Zhang J, Tang Y (2021) Enhanced Removal of sulfonated lignite from oil wastewater with multidimensional MgAl-LDH nanoparticles. Nanomaterials 11:861–880

    CAS  Google Scholar 

  • Zhu YX, Song GL, Wu PP, Huang JF, Zheng DJ (2021) A protective superhydrophobic Mg-Zn-Al LDH film on surface-alloyed magnesium. J Alloy Compd 855:157550

    CAS  Google Scholar 

Download references

Funding

This work is supported by the National Natural Science Foundation of China (Grant Nos. 22078124, 21878119), Program for the Development of Science and Technology of Jilin Province (20210203014SF).

Author information

Authors and Affiliations

Authors

Contributions

Si Wu: conceptualization, methodology, data curation, investigation, writing—original Draft; Huicong Liang: software, formal analysis; Bingyan Xu: formal analysis, investigation; Qi Zhang: formal analysis, data curation; Hougang Fan: validation, investigation; Jingshu Wang: visualization, supervision; Qiang Han: validation, investigation; Ming Gao: writing—review & editing; Jinghai Yang: funding acquisition, project administration; Jihui Lang: funding acquisition, resources, writing—review & editing.

Corresponding author

Correspondence to Jihui Lang.

Ethics declarations

Ethics approval

There are no ethical issues involved in this work and no harm will be caused to individual organisms.

Consent to participate

All authors have consented to participate in submitting this manuscript to this journal.

Consent for publication

All authors have consented to publish this paper in this journal.

Competing interests

The authors declare no competing interests.

Additional information

Responsible Editor: Ricardo A. Torres-Palma

Publisher's note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary Information

Below is the link to the electronic supplementary material.

Supplementary file1 (DOCX 1047 KB)

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.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Wu, S., Liang, H., Xu, B. et al. A co-precipitation route for the preparation of eco-friendly Cu-Al-layered double hydroxides with efficient tetracycline degradation. Environ Sci Pollut Res 30, 99412–99426 (2023). https://doi.org/10.1007/s11356-023-29345-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-023-29345-4

Keywords

Navigation