Journal of Sol-Gel Science and Technology

, Volume 80, Issue 1, pp 215–225 | Cite as

Synthesis of zeolite Y from diatomite and its modification by dimethylglyoxime for the removal of Ni(II) from aqueous solution

  • Shaoqing Zhang
  • Miao Cui
  • Yifu Zhang
  • Zhihui Yu
  • Changgong Meng
Original Paper: Sol-gel and hybrid materials with surface modification for applications


Zeolite Y was obtained from diatomite in a template-free system, and the product was modified by dimethylglyoxime. Characterization studies indicate that the DMG molecules were loaded onto both the exterior surfaces and channels of the zeolite Y during the modification process. Removal of Ni(II) by modified samples was investigated in batch procedure, and it was found that the modified zeolite Y has a very high capacity. The effects of various parameters such as sorbent content, contact time, concentration of nickel solution, pH and selectivity were discussed. The best removal efficiency was observed by Y-DMG at the following experimental conditions: Y-DMG dosage: 2 g L−1, CNi(II): 100 mg L−1 and contact time: 9 h. The Y-DMG sorbent shows good efficiency for the removal of nickel in the presence of different multivalent cations. Adsorption kinetics based on the pseudo-second-order rate equation indicates that the rate-limiting step involves chemical reaction. Adsorption isotherms of Ni(II) ions obey Langmuir equation which indicates the monolayer sorption of Ni(II). The results of thermodynamic parameters of Ni(II) on Y-DMG indicate the process was endothermic and spontaneous.

Graphical Abstract


Ni(II) removal Diatomite Zeolite Dimethylglyoxime Sorption 



This work was partially supported by the National Natural Science Foundation of China (Grant No. 21271037) and Science research project of Liaoning Province Education Department (L2015123).


  1. 1.
    Shahbazi A, Younesi H, Badiei A (2011) Functionalized SBA-15 mesoporous silica by melamine-based dendrimer amines for adsorptive characteristics of Pb(II), Cu(II) and Cd(II) heavy metal ions in batch and fixed bed column. Chem Eng J 168(2):505–518CrossRefGoogle Scholar
  2. 2.
    Bhattacharyya KG, Gupta SS (2008) Influence of acid activation on adsorption of Ni(II) and Cu(II) on kaolinite and montmorillonite: kinetic and thermodynamic study. Chem Eng J 136(1):1–13CrossRefGoogle Scholar
  3. 3.
    Nezamzadeh-Ejhieh A, Kabiri-Samani M (2013) Effective removal of Ni(II) from aqueous solutions by modification of nano particles of clinoptilolite with dimethylglyoxime. J Hazard Mater 260:339–349CrossRefGoogle Scholar
  4. 4.
    Argun ME (2008) Use of clinoptilolite for the removal of nickel ions from water: kinetics and thermodynamics. J Hazard Mater 150(3):587–595CrossRefGoogle Scholar
  5. 5.
    Ren Y et al (2011) Graphene/δ-MnO2 composite as adsorbent for the removal of nickel ions from wastewater. Chem Eng J 175:1–7CrossRefGoogle Scholar
  6. 6.
    Khraisheh M, Aldegs Y, McMinn W (2004) Remediation of wastewater containing heavy metals using raw and modified diatomite. Chem Eng J 99(2):177–184CrossRefGoogle Scholar
  7. 7.
    Faghihian H, Amini M, Nezamzadeh A (2005) Cerium uptake by zeolite A synthesized from natural clinoptilolite tuffs. J Radioanal Nucl Chem 264(3):577–582CrossRefGoogle Scholar
  8. 8.
    Alyuz B, Veli S (2009) Kinetics and equilibrium studies for the removal of nickel and zinc from aqueous solutions by ion exchange resins. J Hazard Mater 167(1–3):482–488CrossRefGoogle Scholar
  9. 9.
    Gök Ö et al (2008) Prediction of the kinetics, equilibrium and thermodynamic parameters of adsorption of copper (II) ions onto 8-hydroxy quinoline immobilized bentonite. Colloids Surf, A 317(1):174–185CrossRefGoogle Scholar
  10. 10.
    Katsou E et al (2010) Use of ultrafiltration membranes and aluminosilicate minerals for nickel removal from industrial wastewater. J Membr Sci 360(1–2):234–249CrossRefGoogle Scholar
  11. 11.
    Seneviratne J, Cox JA (2000) Sol–gel materials for the solid phase extraction of metals from aqueous solution. Talanta 52(5):801–806CrossRefGoogle Scholar
  12. 12.
    Shao J et al (2013) Recovery of nickel from aqueous solutions by complexation-ultrafiltration process with sodium polyacrylate and polyethylenimine. J Hazard Mater 244–245:472–477CrossRefGoogle Scholar
  13. 13.
    Franco PE et al (2013) Nickel(II) and zinc(II) removal using Amberlite IR-120 resin: ion exchange equilibrium and kinetics. Chem Eng J 221:426–435CrossRefGoogle Scholar
  14. 14.
    Alemayehu E, Lennartz B (2010) Adsorptive removal of nickel from water using volcanic rocks. Appl Geochem 25(10):1596–1602CrossRefGoogle Scholar
  15. 15.
    Vieira MG et al (2010) Sorption kinetics and equilibrium for the removal of nickel ions from aqueous phase on calcined Bofe bentonite clay. J Hazard Mater 177(1–3):362–371CrossRefGoogle Scholar
  16. 16.
    Miller A, Figueroa L, Wildeman T (2011) Zinc and nickel removal in simulated limestone treatment of mining influenced water. Appl Geochem 26(1):125–132CrossRefGoogle Scholar
  17. 17.
    Duman O, Ayranci E (2010) Attachment of benzo-crown ethers onto activated carbon cloth to enhance the removal of chromium, cobalt and nickel ions from aqueous solutions by adsorption. J Hazard Mater 176(1–3):231–238CrossRefGoogle Scholar
  18. 18.
    Tan XL et al (2008) Characterization of Lin’an montmorillonite and its application in the removal of Ni2+ from aqueous solutions. Radiochim Acta 96(8/2008):487–495CrossRefGoogle Scholar
  19. 19.
    Anari-Anaraki M, Nezamzadeh-Ejhieh A (2015) Modification of an Iranian clinoptilolite nano-particles by hexadecyltrimethyl ammonium cationic surfactant and dithizone for removal of Pb(II) from aqueous solution. J Colloid Interface Sci 440:272–281CrossRefGoogle Scholar
  20. 20.
    Panneerselvam P et al (2009) Removal of nickel (II) from aqueous solutions by adsorption with modified ZSM-5 zeolites. J Chem 6(3):729–736Google Scholar
  21. 21.
    Petrus R, Warchol JK (2005) Heavy metal removal by clinoptilolite. An equilibrium study in multi-component systems. Water Res 39(5):819–830CrossRefGoogle Scholar
  22. 22.
    Kang SY et al (2004) Competitive adsorption characteristics of Co2+, Ni2+, and Cr3+ by IRN-77 cation exchange resin in synthesized wastewater. Chemosphere 56(2):141–147CrossRefGoogle Scholar
  23. 23.
    Erdem E, Karapinar N, Donat R (2004) The removal of heavy metal cations by natural zeolites. J Colloid Interface Sci 280(2):309–314CrossRefGoogle Scholar
  24. 24.
    Lin J, Zhan Y, Zhu Z (2011) Adsorption characteristics of copper (II) ions from aqueous solution onto humic acid-immobilized surfactant-modified zeolite. Colloids Surf, A 384(1–3):9–16CrossRefGoogle Scholar
  25. 25.
    Benhamou A et al (2009) Aqueous heavy metals removal on amine-functionalized Si-MCM-41 and Si-MCM-48. J Hazard Mater 171(1–3):1001–1008CrossRefGoogle Scholar
  26. 26.
    Chandra D, Das SK, Bhaumik A (2010) A fluorophore grafted 2D-hexagonal mesoporous organosilica: excellent ion-exchanger for the removal of heavy metal ions from wastewater. Microporous Mesoporous Mater 128(1–3):34–40CrossRefGoogle Scholar
  27. 27.
    Paul M et al (2010) New organic-inorganic hybrid microporous organosilica having high metal ion adsorption capacity. Phys Chem Chem Phys 12(32):9389–9394CrossRefGoogle Scholar
  28. 28.
    Gazda DB, Fritz JS, Porter MD (2004) Determination of nickel (II) as the nickel dimethylglyoxime complex using colorimetric solid phase extraction. Anal Chim Acta 508(1):53–59CrossRefGoogle Scholar
  29. 29.
    Banks CV, Anderson S (1962) Nickel–nickel bond in nickel dimethylglyoxime. J Am Chem Soc 84(8):1486–1487CrossRefGoogle Scholar
  30. 30.
    Sharp AG, Wakefield DB (1957) The basis of the selectivity of dimethylglyoxime as a reagent in gravimetric analysis. J Chem Soc 281–285. doi: 10.1039/jr9570000281
  31. 31.
    Yang S et al (2009) Sorption of Ni(II) on GMZ bentonite: effects of pH, ionic strength, foreign ions, humic acid and temperature. Appl Radiat Isotopes 67(9):1600–1608CrossRefGoogle Scholar
  32. 32.
    Heidari A, Younesi H, Mehraban Z (2009) Removal of Ni(II), Cd(II), and Pb(II) from a ternary aqueous solution by amino functionalized mesoporous and nano mesoporous silica. Chem Eng J 153(1–3):70–79CrossRefGoogle Scholar
  33. 33.
    Ahmed AH, Thabet MS (2011) Metallo-hydrazone complexes immobilized in zeolite Y: synthesis, identification and acid violet-1 degradation. J Mol Struct 1006(1–3):527–535CrossRefGoogle Scholar
  34. 34.
    Hihara G (2004) Mechanochemical syntheses of complexes through solid?solid reactions of divalent transition metal salts [Ni(II) or Cu(II)] with dimethylglyoxime. Solid State Ionics 172(1–4):221–223CrossRefGoogle Scholar
  35. 35.
    Qureshi A et al (2008) Modification of polymer composite films using 120 MeV Ni10+ ions. Nucl Instrum Methods Phys Res Sect B 266(8):1775–1779CrossRefGoogle Scholar
  36. 36.
    Liang Z et al (2008) Stepwise growth of melamine-based dendrimers into mesopores and their CO2 adsorption properties. Microporous Mesoporous Mater 111(1):536–543CrossRefGoogle Scholar
  37. 37.
    Cardoso WS et al (2008) Nickel-dimethylglyoxime complex modified graphite and carbon paste electrodes: preparation and catalytic activity towards methanol/ethanol oxidation. J Appl Electrochem 39(1):55–64CrossRefGoogle Scholar
  38. 38.
    Xavier K, Chacko J, Yusuff KM (2004) Zeolite-encapsulated Co(II), Ni(II) and Cu(II) complexes as catalysts for partial oxidation of benzyl alcohol and ethylbenzene. Appl Catal A 258(2):251–259CrossRefGoogle Scholar
  39. 39.
    Shaker SA (2010) Preparation and spectral properties of mixed-ligand complexes of VO(IV), Ni(II), Zn(II), Pd(II), Cd(II) and Pb(II) with dimethylglyoxime and N-acetylglycine. J Chem 7(S1):S580–S586Google Scholar
  40. 40.
    Osunlaja A, Ndahi N, Ameh J (2009) Synthesis, physico-chemical and antimicrobial properties of Co(II), Ni(II) and Cu(II) mixed-ligand complexes of dimethylglyoxime-Part I. Afr J Biotechnol 8(1):4–11Google Scholar
  41. 41.
    Blinc R, Hadži D (1958) Infrared spectra and hydrogen bonding in the nickel–dimethylglyoxime and related complexes. J Chem Soc 4536–4540. doi: 10.1039/JR9580004536
  42. 42.
    Anilan B, Gedikbey T, Tunali Akar S (2010) Determination of copper in water samples after solid-phase extraction using dimethylglyoxime-modified silica. CLEAN–Soil, Air, Water 38(4):344–352CrossRefGoogle Scholar
  43. 43.
    Al-Thabaiti S et al (1998) Kinetics of thermal decomposition of nickel dimethylglyoxime. JKAU Sci 10:103–113CrossRefGoogle Scholar
  44. 44.
    Dean JA (1985) Lange’s handbook of chemistry. McGraw-Hill, New YorkGoogle Scholar
  45. 45.
    Zeng Y et al (2010) Removal of chromate from water using surfactant modified Pohang clinoptilolite and Haruna chabazite. Desalination 257(1–3):102–109CrossRefGoogle Scholar
  46. 46.
    Baral SS, Das SN, Rath P (2006) Hexavalent chromium removal from aqueous solution by adsorption on treated sawdust. Biochem Eng J 31(3):216–222CrossRefGoogle Scholar
  47. 47.
    Chunfeng W et al (2009) Evaluation of zeolites synthesized from fly ash as potential adsorbents for wastewater containing heavy metals. J Environ Sci 21(1):127–136CrossRefGoogle Scholar
  48. 48.
    Inglezakis VJ, Stylianou M, Loizidou M (2010) Ion exchange and adsorption equilibrium studies on clinoptilolite, bentonite and vermiculite. J Phys Chem Solids 71(3):279–284CrossRefGoogle Scholar
  49. 49.
    Zhang H et al (2010) Study of (6)(3)Ni adsorption on NKF-6 zeolite. J Environ Radioact 101(12):1061–1069CrossRefGoogle Scholar
  50. 50.
    Tao YF et al (2010) Trapping the lead ion in multi-components aqueous solution by natural clinoptilolite. J Hazard Mater 180(1–3):282–288CrossRefGoogle Scholar
  51. 51.
    Hui KS, Chao CY, Kot SC (2005) Removal of mixed heavy metal ions in wastewater by zeolite 4A and residual products from recycled coal fly ash. J Hazard Mater 127(1–3):89–101CrossRefGoogle Scholar
  52. 52.
    Saeed A, Akhter M, Iqbal M (2005) Removal and recovery of heavy metals from aqueous solution using papaya wood as a new biosorbent. Sep Purif Technol 45(1):25–31CrossRefGoogle Scholar
  53. 53.
    Sangi MR et al (2008) Removal and recovery of heavy metals from aqueous solution using Ulmus carpinifolia and Fraxinus excelsior tree leaves. J Hazard Mater 155(3):513–522CrossRefGoogle Scholar
  54. 54.
    Ghiaci M et al (2004) Equilibrium isotherm studies for the sorption of benzene, toluene, and phenol onto organo-zeolites and as-synthesized MCM-41. Sep Purif Technol 40(3):217–229CrossRefGoogle Scholar
  55. 55.
    Ibrahim HS, Jamil TS, Hegazy EZ (2010) Application of zeolite prepared from Egyptian kaolin for the removal of heavy metals: II. Isotherm models. J Hazard Mater 182(1–3):842–847CrossRefGoogle Scholar
  56. 56.
    Zeledón-Toruño Z, Lao-Luque C, Solé-Sardans M (2005) Nickel and copper removal from aqueous solution by an immature coal (leonardite): effect of pH, contact time and water hardness. J Chem Technol Biotechnol 80(6):649–656CrossRefGoogle Scholar
  57. 57.
    Chen C et al (2007) Imaging of humic acid macromolecular structures observed by atomic force microscopy and scanning electron microscope. Colloid Surf A Physicochem Eng Asp 302:121–125CrossRefGoogle Scholar
  58. 58.
    Nibou D et al (2010) Adsorption of Zn2+ ions onto NaA and NaX zeolites: kinetic, equilibrium and thermodynamic studies. J Hazard Mater 173(1–3):637–646CrossRefGoogle Scholar
  59. 59.
    Sprynskyy M (2009) Solid–liquid–solid extraction of heavy metals (Cr, Cu, Cd, Ni and Pb) in aqueous systems of zeolite-sewage sludge. J Hazard Mater 161(2–3):1377–1383CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media New York 2016

Authors and Affiliations

  • Shaoqing Zhang
    • 1
  • Miao Cui
    • 1
  • Yifu Zhang
    • 1
  • Zhihui Yu
    • 1
  • Changgong Meng
    • 1
  1. 1.School of ChemistryDalian University of TechnologyDalianChina

Personalised recommendations