Skip to main content
SpringerLink
Log in

Synthesis of Three-Dimensional Hierarchical Flower-Like Mg–Al Layered Double Hydroxides with Excellent Adsorption Performance for Organic Anionic Dyes

  • Research Article
  • Published:
Transactions of Tianjin University Aims and scope Submit manuscript

Abstract

In this work, a facile and effective strategy to prepare three-dimensional (3D) hierarchical flower-like Mg–Al layered double hydroxides (3D-LDH) was developed via a one-step double-drop coprecipitation method using γ-Al2O3 particles as a template. The characterization and experimental results showed that the calcined product, 3D-LDO, features a large specific surface area of 204.2 m2/g, abundant active sites, and excellent adsorption performance for Congo red (CR), methyl orange (MO), and methyl blue (MB). The maximum adsorption capacities of 3D-LDO for CR, MO, and MB were 1428.6, 476.2, and 1666.7 mg/g, respectively; such performance is superior to that of most reported adsorbents. The adsorption mechanism of organic anionic dyes by 3D-LDO was extensively investigated and attributed to surface adsorption, the memory effect of 3D-LDO, and the unique 3D hierarchical flower-like structure of the adsorbent. Recycling performance tests revealed that 3D-LDO has satisfactory reusability for the three organic anionic dyes.

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

Access this article

Log in via an institution

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

Instant access to the full article PDF.

Institutional subscriptions

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
Fig. 16
Fig. 17
Fig. 18

Similar content being viewed by others

References

  1. Yang HW, Bai LJ, Wei DL et al (2019) Ionic self-assembly of poly(ionic liquid)-polyoxometalate hybrids for selective adsorption of anionic dyes. Chem Eng J 358:850–859

    Article  Google Scholar 

  2. Zhang WK, Liang Y, Wang JW et al (2019) Ultrasound-assisted adsorption of Congo red from aqueous solution using MgAlCO3 layered double hydroxide. Appl Clay Sci 174:100–109

    Article  Google Scholar 

  3. Ling FL, Fang L, Lu Y et al (2016) A novel CoFe layered double hydroxides adsorbent: high adsorption amount for methyl orange dye and fast removal of Cr(VI). Microporous Mesoporous Mater 234:230–238

    Article  Google Scholar 

  4. Lau WJ, Ismail AF (2009) Polymeric nanofiltration membranes for textile dye wastewater treatment: preparation, performance evaluation, transport modelling, and fouling control: a review. Desalination 245(1–3):321–348

    Article  Google Scholar 

  5. Ma X, Chen PL, Zhou M et al (2017) Tight ultrafiltration ceramic membrane for separation of dyes and mixed salts (both NaCl/Na2SO4) in textile wastewater treatment. Ind Eng Chem Res 56(24):7070–7079

    Article  Google Scholar 

  6. Cotillas S, Llanos J, Cañizares P et al (2018) Removal of Procion Red MX-5B dye from wastewater by conductive-diamond electrochemical oxidation. Electrochim Acta 263:1–7

    Article  Google Scholar 

  7. Türgay O, Ersöz G, Atalay S et al (2011) The treatment of azo dyes found in textile industry wastewater by anaerobic biological method and chemical oxidation. Sep Purif Technol 79(1):26–33

    Article  Google Scholar 

  8. Zargari S, Rahimi R, Ghaffarinejad A et al (2016) Enhanced visible light photocurrent response and photodegradation efficiency over TiO2–graphene nanocomposite pillared with tin porphyrin. J Colloid Interface Sci 466:310–321

    Article  Google Scholar 

  9. Yao W, Yu SJ, Wang J et al (2017) Enhanced removal of methyl orange on calcined glycerol-modified nanocrystallined Mg/Al layered double hydroxides. Chem Eng J 307:476–486

    Article  Google Scholar 

  10. Extremera R, Pavlovic I, Pérez MR et al (2012) Removal of acid orange 10 by calcined Mg/Al layered double hydroxides from water and recovery of the adsorbed dye. Chem Eng J 213:392–400

    Article  Google Scholar 

  11. Lu L, Li J, Ng DHL et al (2017) Synthesis of novel hierarchically porous Fe3O4@MgAl–LDH magnetic microspheres and its superb adsorption properties of dye from water. J Ind Eng Chem 46:315–323

    Article  Google Scholar 

  12. Patra S, Roy E, Madhuri R et al (2016) Agar based bimetallic nanoparticles as high-performance renewable adsorbent for removal and degradation of cationic organic dyes. J Ind Eng Chem 33:226–238

    Article  Google Scholar 

  13. Yagub MT, Sen TK, Afroze S et al (2014) Dye and its removal from aqueous solution by adsorption: a review. Adv Colloid Interface Sci 209:172–184

    Article  Google Scholar 

  14. Zheng YQ, Cheng B, You W et al (2019) 3D hierarchical graphene oxide-NiFe LDH composite with enhanced adsorption affinity to Congo red, methyl orange and Cr(VI) ions. J Hazard Mater 369:214–225

    Article  Google Scholar 

  15. Demirbas A (2009) Agricultural based activated carbons for the removal of dyes from aqueous solutions: a review. J Hazard Mater 167(1–3):1–9

    Article  Google Scholar 

  16. Zhou CJ, Wu QL, Lei TZ et al (2014) Adsorption kinetic and equilibrium studies for methylene blue dye by partially hydrolyzed polyacrylamide/cellulose nanocrystal nanocomposite hydrogels. Chem Eng J 251:17–24

    Article  Google Scholar 

  17. Jin XY, Yu B, Chen ZL et al (2014) Adsorption of Orange II dye in aqueous solution onto surfactant-coated zeolite: characterization, kinetic and thermodynamic studies. J Colloid Interface Sci 435:15–20

    Article  Google Scholar 

  18. Vimonses V, Lei SM, Jin B et al (2009) Kinetic study and equilibrium isotherm analysis of Congo Red adsorption by clay materials. Chem Eng J 148(2–3):354–364

    Article  Google Scholar 

  19. Zeng SY, Duan SX, Tang RF et al (2014) Magnetically separable Ni0.6Fe2.4O4 nanoparticles as an effective adsorbent for dye removal: synthesis and study on the kinetic and thermodynamic behaviors for dye adsorption. Chem Eng J 258:218–228

    Article  Google Scholar 

  20. Hu HJ, Liu JY, Xu ZH et al (2019) Hierarchical porous Ni/Co-LDH hollow dodecahedron with excellent adsorption property for Congo red and Cr(VI) ions. Appl Surf Sci 478:981–990

    Article  Google Scholar 

  21. Yu JY, Fan GL, Yang Y et al (2014) Multi-level three-dimensional Mg-Al layered double hydroxide hierarchical microstructures with enhanced basic catalytic property. J Colloid Interface Sci 432:1–9

    Article  Google Scholar 

  22. Liu P, Derchi M, Hensen EJM (2013) Synthesis of glycerol carbonate by transesterification of glycerol with dimethyl carbonate over MgAl mixed oxide catalysts. Appl Catal A: Gen 467:124–131

    Article  Google Scholar 

  23. dos Santos RMM, Gonçalves RGL, Constantino VRL et al (2017) Adsorption of Acid Yellow 42 dye on calcined layered double hydroxide: effect of time, concentration, pH and temperature. Appl Clay Sci 140:132–139

    Article  Google Scholar 

  24. Baskaran T, Christopher J, Sakthivel A (2015) Progress on layered hydrotalcite (HT) materials as potential support and catalytic materials. RSC Adv 5(120):98853–98875

    Article  Google Scholar 

  25. Zaghouane-Boudiaf H, Boutahala M, Arab L (2012) Removal of methyl orange from aqueous solution by uncalcined and calcined MgNiAl layered double hydroxides (LDHs). Chem Eng J 187:142–149

    Article  Google Scholar 

  26. Li ZC, Yang BJ, Zhang SN et al (2014) A novel approach to hierarchical sphere-like ZnAl-layered double hydroxides and their enhanced adsorption capability. J Mater Chem A 2(26):10202

    Article  Google Scholar 

  27. Li J, Zhang N, Ng DHL (2015) Synthesis of a 3D hierarchical structure of γ-AlO(OH)/Mg–Al-LDH/C and its performance in organic dyes and antibiotics adsorption. J Mater Chem A 3(42):21106–21115

    Article  Google Scholar 

  28. Dong T, Zhang X, Li M et al (2018) Hierarchical flower-like Ni–Co layered double hydroxide nanostructures: synthesis and super performance. Inorg Chem Front 5(12):3033–3041

    Article  Google Scholar 

  29. Xu J, Deng HH, Song JX et al (2017) Synthesis of hierarchical flower-like Mg2Al–Cl layered double hydroxide in a surfactant-free reverse microemulsion. J Colloid Interface Sci 505:816–823

    Article  Google Scholar 

  30. Zhang P, Ouyang SD, Li P et al (2019) Enhanced removal of ionic dyes by hierarchical organic three-dimensional layered double hydroxide prepared via soft-template synthesis with mechanism study. Chem Eng J 360:1137–1149

    Article  Google Scholar 

  31. Zong YT, Li KT, Tian R et al (2018) Highly dispersed layered double oxide hollow spheres with sufficient active sites for adsorption of methyl blue. Nanoscale 10(48):23191–23197

    Article  Google Scholar 

  32. Li L, Ma RZ, Iyi N et al (2006) Hollow nanoshell of layered double hydroxide. Chem Commun 29:3125

    Article  Google Scholar 

  33. Li B, He J (2008) Multiple effects of dodecanesulfonate in the crystal growth control and morphosynthesis of layered double hydroxides. J Phys Chem C 112(29):10909–10917

    Article  Google Scholar 

  34. He S, Zhao YF, Wei M et al (2012) Fabrication of hierarchical layered double hydroxide framework on aluminum foam as a structured adsorbent for water treatment. Ind Eng Chem Res 51(1):285–291

    Article  Google Scholar 

  35. Shao MF, Ning FY, Zhao YF et al (2012) Core–shell layered double hydroxide microspheres with tunable interior architecture for supercapacitors. Chem Mater 24(6):1192–1197

    Article  Google Scholar 

  36. Sun HX, Chu ZY, Hong DH et al (2016) Three-dimensional hierarchical flower-like Mg-Al-layered double hydroxides: fabrication, characterization and enhanced sensing properties to NOx at room temperature. J Alloyf Compd 658:561–568

    Article  Google Scholar 

  37. Bo LF, Li QR, Wang YH et al (2016) Adsorptive removal of fluoride using hierarchical flower-like calcined Mg-Al layered double hydroxides. Environ Prog Sustain Energy 35(5):1420–1429

    Article  Google Scholar 

  38. Yu XY, Luo T, Jia Y et al (2012) Three-dimensional hierarchical flower-like Mg–Al-layered double hydroxides: highly efficient adsorbents for As(v) and Cr(vi) removal. Nanoscale 4(11):3466

    Article  Google Scholar 

  39. Sun YL, Gao X, Yang N et al (2019) Morphology-controlled synthesis of three-dimensional hierarchical flowerlike Mg–Al layered double hydroxides with enhanced catalytic activity for transesterification. Ind Eng Chem Res 58(19):7937–7947

    Article  Google Scholar 

  40. Wu GD, Wang XL, Chen B et al (2007) Fluorine-modified mesoporous Mg-Al mixed oxides: mild and stable base catalysts for O-methylation of phenol with dimethyl carbonate. Appl Catal A: Gen 329:106–111

    Article  Google Scholar 

  41. Nethravathi C, Viswanath B, Sebastian M et al (2010) Exfoliation of α-hydroxides of nickel and cobalt in water. J Colloid Interface Sci 345(1):109–115

    Article  Google Scholar 

  42. Herrero M, Benito P, Labajos FM et al (2007) Nanosize cobalt oxide-containing catalysts obtained through microwave-assisted methods. Catal Today 128(3–4):129–137

    Article  Google Scholar 

  43. Zheng YM, Li N, Zhang WD (2012) Preparation of nanostructured microspheres of Zn-Mg-Al layered double hydroxides with high adsorption property. Colloids Surf A: Physicochem Eng Asp 415:195–201

    Article  Google Scholar 

  44. Kloprogge J, Frost RL (1999) Fourier transform infrared and Raman spectroscopic study of the local structure of Mg-, Ni-, and Co-hydrotalcites. J Solid State Chem 146(2):506–515

    Article  Google Scholar 

  45. Pooralhossini J, Ghaedi M, Zanjanchi MA et al (2017) Ultrasonically assisted removal of Congo Red, Phloxine B and Fast green FCF in ternary mixture using novel nanocomposite following their simultaneous analysis by derivative spectrophotometry. Ultrason Sonochemistry 37:452–463

    Article  Google Scholar 

  46. Cao CY, Liang CH, Yin Y et al (2017) Thermal activation of serpentine for adsorption of cadmium. J Hazard Mater 329:222–229

    Article  Google Scholar 

  47. Zhang ML, Yao QF, Lu C et al (2014) Layered double hydroxide–carbon dot composite: high-performance adsorbent for removal of anionic organic dye. ACS Appl Mater Interfaces 6(22):20225–20233

    Article  Google Scholar 

  48. Wu FC, Tseng RL, Juang RS (2009) Characteristics of Elovich equation used for the analysis of adsorption kinetics in dye-chitosan systems. Chem Eng J 150(2–3):366–373

    Article  Google Scholar 

  49. Nethaji S, Sivasamy A, Mandal AB (2013) Preparation and characterization of corn cob activated carbon coated with nano-sized magnetite particles for the removal of Cr(VI). Bioresour Technol 134:94–100

    Article  Google Scholar 

  50. Pourfaraj R, Fatemi SJ, Kazemi SY et al (2017) Synthesis of hexagonal mesoporous MgAl LDH nanoplatelets adsorbent for the effective adsorption of Brilliant Yellow. J Colloid Interface Sci 508:65–74

    Article  Google Scholar 

  51. Shamsayei M, Yamini Y, Asiabi H (2018) Fabrication of zwitterionic histidine/layered double hydroxide hybrid nanosheets for highly efficient and fast removal of anionic dyes. J Colloid Interface Sci 529:255–264

    Article  Google Scholar 

  52. Qiao Y, Li QR, Chi HJ et al (2018) Methyl blue adsorption properties and bacteriostatic activities of Mg-Al layer oxides via a facile preparation method. Appl Clay Sci 163:119–128

    Article  Google Scholar 

  53. Li J, Xu L, Sun PP et al (2017) Novel application of red mud: facile hydrothermal-thermal conversion synthesis of hierarchical porous AlOOH and Al2O3 microspheres as adsorbents for dye removal. Chem Eng J 321:622–634

    Article  Google Scholar 

  54. Sharma P, Hussain N, Borah DJ et al (2013) Kinetics and adsorption behavior of the methyl blue at the graphene oxide/reduced graphene oxide nanosheet–water interface: a comparative study. J Chem Eng Data 58(12):3477–3488

    Article  Google Scholar 

  55. Hájek M, Kutálek P, Smoláková L et al (2015) Transesterification of rapeseed oil by Mg-Al mixed oxides with various Mg/Al molar ratio. Chem Eng J 263:160–167

    Article  Google Scholar 

  56. Wang LX, Li JC, Wang ZT et al (2013) Low-temperature hydrothermal synthesis of α-Fe/Fe3O4nanocomposite for fast Congo red removal. Dalton Trans 42(7):2572–2579

    Article  Google Scholar 

  57. Yang SX, Wang LY, Zhang XD et al (2015) Enhanced adsorption of Congo red dye by functionalized carbon nanotube/mixed metal oxides nanocomposites derived from layered double hydroxide precursor. Chem Eng J 275:315–321

    Article  Google Scholar 

  58. Zhou QQ, Chen FF, Wu W et al (2016) Reactive orange 5 removal from aqueous solution using hydroxyl ammonium ionic liquids/layered double hydroxides intercalation composites. Chem Eng J 285:198–206

    Article  Google Scholar 

Download references

Acknowledgements

This study was supported by the National Key R&D Program of China (No. 2017YFB0602702-02).

Author information

Authors and Affiliations

  1. School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China

    Luhong Zhang, Dandan Guo, Xiaowei Tantai, Bin Jiang, Yongli Sun & Na Yang

Authors
  1. Luhong Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Dandan Guo
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xiaowei Tantai
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Bin Jiang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Yongli Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Na Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Na Yang.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 383 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, L., Guo, D., Tantai, X. et al. Synthesis of Three-Dimensional Hierarchical Flower-Like Mg–Al Layered Double Hydroxides with Excellent Adsorption Performance for Organic Anionic Dyes. Trans. Tianjin Univ. 27, 394–408 (2021). https://doi.org/10.1007/s12209-020-00249-5

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12209-020-00249-5

Keywords

Search

Navigation