Skip to main content
Log in

Green Synthesis of the Metakaolin/slag Based Geopolymer for the Effective Removal of Methylene Blue and Pb (II)

  • Original Paper
  • Published:
Silicon Aims and scope Submit manuscript

Abstract

In this paper, metakaolin with varying amounts of slag were used to prepare metakaolin/slag based geopolymer adsorbents for removal of methylene blue (MB) and Lead ions (Pb2+). XRD, SEM, FT-IR and BET methods were used to analyze the phase, structure and morphology of the samples. The effects of slag addition, adsorbent dosage, pH value of Pb2+ solution, initial mass concentration, contact time between sample and solution, experimental temperature on the adsorption properties of the metakaolin/slag based geopolymers were explored. Experiments have shown that the metakaolin/slag based geopolymers are mainly consisted of amorphous phases. The structure of the samples does not change obviously with the increase of the amount of slag addition. The kinetic adsorption process of the metakaolin/slag based geopolymer adsorbents for MB and Pb2+ are fitted to the pseudo-second-order model, and followed by the Langmuir isotherm model. The adsorption process of the geopolymer adsorbents occurs spontaneously with exothermic character. The type of metakaolin/slag based geopolymer has good adsorption capacity for MB and Pb2+, which has potential application in wastewater treatment.

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.

Similar content being viewed by others

Data Availability

The data related to the work were published in this article.

References

  1. Ariffin N, Abdullah M, Postawa P, Zamree Abd Rahim S, Mohd Arif Zainol MRR, Jaya RP, Sliwa A, Omar MF, Wyslocki,Bloch JJK, Nabialek M (2021) Effect of aluminium powder on kaolin-based geopolymer characteristic and removal of Cu2+. Materials 14(4):814

    Article  CAS  Google Scholar 

  2. Sibongile NC, David SN, Bobby NE (2020) Adsorption studies of methylene blue and lead ions from aqueous solution by using mesoporous coral limestones. S Afr J Chem Eng 34:151–157

  3. Paul D (2017) Research on heavy metal pollution of river Ganga: A review. Annals of Agrarian Science 15(2):278–286

  4. Daud NAA, Shamsuddin MR, Pradanawati SA (2021) Synthesis and characterization of fly ash-based geopolymer membrane for methylene blue dye removal. IOP Conf Ser Earth Environ Sci 765(1):012081

  5. Rafatullah M, Sulaiman O, Hashim R, Ahmad A (2010) Adsorption of methylene blue on low-cost adsorbents: a review. J Hazard Mater 177(1–3):70–80

  6. Allafchian A, Mousavi ZS, Hosseini SS (2019) Application of cress seed musilage magnetic nanocomposites for removal of methylene blue dye from water. Int J Biol Macromol 136:199–208

  7. Liu Y, Yan C, Zhang Z, Wang H, Zhou S, Zhou W (2016) A comparative study on fly ash, geopolymer and faujasite block for Pb removal from aqueous solution. Fuel 185:181–189

  8. Maleki A, Hajizadeh Z, Sharifi V, Emdadi Z (2019) A green, porous and eco-friendly magnetic geopolymer adsorbent for heavy metals removal from aqueous solutions. J Clean Prod 215:1233–1245

  9. Elettra P, Matteo M, Annalisa NM, Elena L, Valentina M (2020) Ice-templated geopolymer beads for dye remova. J Colloid Interf Sci 572:364–373

  10. Mustakim SM, Das SK, Mishra J, Mishra J, Aftab A, Alomayri TS, Assaedi HS, Kaze CR (2020) Improvement in fresh, mechanical and microstructural properties of fly ash- blast furnace slag sased geopolymer concrete by dddition of nano and micro silica. Silicon 13:2415–2428

  11. Ojha A, Aggarwal P (2021) Fly ash based geopolymer concrete: a comprehensive review. Silicon. https://doi.org/10.1007/S12633-021-01044-0

  12. Juengsuwattananon K, Winnefeld F, Chindaprasirt P, Pimraksa K (2019) Correlation between initial SiO2/Al2O3, Na2O/Al2O3, Na2O/SiO2 and H2O/Na2O ratios on phase and microstructure of reaction products of metakaolin-rice husk ash geopolymer. Constr Build Mater 226:406–417

  13. Thant N, Soe ZN (2019) The effect of dosage and modulus of activator on the strength of alkali activated slag and fly ash based on geopolymer mortar. J Trend Sci Res Dev 3(5):2220–2224

    CAS  Google Scholar 

  14. Phummiphan I, Horpibulsuk S, Rachan R, Arulrajah A, Shen SL, Chindaprasirt P (2018) High calcium fly ash geopolymer stabilized lateritic soil and granulated blast furnace slag blends as a pavement base material. J Hazard Mater 341:257–267

  15. Singh NB, Middendorf B (2020) Geopolymers as an alternative to Portland cement: An overview. Constr Build Mater 237:117455

  16. Shuai Q, Xu Z, Yao Z, Chen X, Jiang Z, Peng X, An R, Li Y, Jiang X, Li H (2020) Fire resistance of phosphoric acid-based geopolymer foams fabricated from metakaolin and hydrogen peroxide. Mater Lett 263:127228

  17. Giroudon M, Peyre Lavigne M, Patapy C, Bertron A (2017) Blast-furnace slag cement and metakaolin based geopolymer as construction materials for liquid anaerobic digestion structures: Interactions and biodeterioration mechanisms. Sci Total Environ 750:141518

  18. Linda Bih N, Aboubakar Mahamat A, Bidossèssi Hounkpè J, Azikiwe Onwualu P, Boakye EE (2021) The effect of polymer waste addition on the compressive strength and water absorption of geopolymer ceramics. Appl Sci Basel 11(8):3540–3553

  19. Hua P, Sellaoui L, Franco D, Netto MS, Luiz Dotto G, Bajahzar A, Belmabrouk H, Bonilla-Petriciolet A, Li Z (2020) Adsorption of acid green and procion red on a magnetic geopolymer based adsorbent: Experiments, characterization and theoretical treatment. Chem Eng J 383:123113

  20. Chen F, Wang K, Shao L, Muhammad Y, Wei Y, Gao F, Wang X, Cui X (2019) Synthesis of Fe2O3-modified porous geopolymer microspheres for highly selective adsorption and solidification of F from waste-water. Compos Part B-Eng 178:107497

  21. Njimou JR, Pengou M, Tchakoute HK, Sieugaing Tamwa M, Tizaoui C, Fannang U, Lemougna PN, Nanseu-Njiki CP, Ngameni E (2021) Removal of lead ions from aqueous solution using phosphate‐based geopolymer cement composite. J Chem Technol Biot 96(5):1358–1369

  22. Kim SH, Chung H, Jeong S, Nam K (2021) Identification of pH-dependent removal mechanisms of lead and arsenic by basic oxygen furnace slag: Relative contribution of precipitation and adsorption. J Clean Prod 279:123451

  23. Li F, Yang Z, Zheng A, Li S (2021) Properties of modified engineered geopolymer composites incorporating multi-walled carbon Nanotubes (MWCNTs) and granulated blast furnace Slag (GBFS). Ceram Int 46:14244–14259

  24. Gan L, Zhang C, Shangguan F, Li X (2012) A Differential Scanning Calorimetry Method for Construction of Continuous Cooling Transformation Diagram of Blast Furnace Slag. Metall Mater Trans B 43:460–467

  25. Rashad AM, Sadek DM (2020) Behavior of alkali-activated slag pastes blended with waste rubber powder under the effect of freeze/thaw cycles and severe sulfate attack. Constr Build Mater 265:120716

  26. Mayhoub OA, Nasr E-S A R, Ali Y, Kohail M (2021) Properties of slag based geopolymer reactive powder concrete. Ain Shams Eng J 12(1):99–105

    Article  Google Scholar 

  27. Yasipourtehrani S, Strezov V, Kan T, Evans T (2021) Investigation of dye removal capability of blast furnace slag in wastewater treatment. Sustainability 13(4):1970–1986

  28. Sarkar C, Basu JK, Samanta AN (2017) Removal of Ni2+ ion from waste water by geopolymeric adsorbent derived from LD Slag. J Water Process Eng 17:237–244

    Article  Google Scholar 

  29. Zhou S, Zhou S, Zhang J, Tan X, Chen D (2020) Relationship between moisture transportation, efflorescence and structure degradation in fly ash/slag geopolymer. Materials 13(23):5550–5565

  30. Wu J, Zhang Z, Zhang Y, Li D (2018) Preparation and characterization of ultra-lightweight foamed geopolymer (UFG) based on fly ash-metakaolin blends. Constr Build Mater 168:771–779

  31. Zhang P, Gao Z, Wang J, Guo J, Hu S, Ling Y (2020) Properties of fresh and hardened fly ash/slag based geopolymer concrete: A review. J Clean Prod 270:122389

  32. Zhu H, Liang G, Li H, Wu Q, Zhang C, Yin Z, Hua S (2021) Insights to the sulfate resistance and microstructures of alkali-activated metakaolin/slag pastes. Appl Clay Sci 202:105968

  33. Peng H, Cui C, Liu Z, Cai CS, Liu Y (2019) Synthesis and reaction mechanism of an alkali-activated metakaolin-slag composite system at room temperature. J Mater Civil Eng 31(1):04018345

    Article  CAS  Google Scholar 

  34. Chen X, Guo Y, Ding S, Zhang H, Xia F, Wang J, Zhou M (2019) Utilization of red mud in geopolymer-based pervious concrete with function of adsorption of heavy metal ions. J Clean Prod 207:789–800

  35. Lei H, Muhammad Y, Wang K, Yi M, He C, Wei Y, Fujita T (2021) Facile fabrication of metakaolin/slag-based zeolite microspheres (M/SZMs) geopolymer for the efficient remediation of Cs+ and Sr2+ from aqueous media. J Hazard Mater 406:124292

  36. Yan S, Wang Q, Liu J, Huo W, Yang J, Huang Y, Synthesis (2019) Characterization and adsorption properties of low-cost porous calcined dolomite microspheres for removal of dyes. J Wuhan Univ Technol 34(3):507–515

    Article  CAS  Google Scholar 

  37. Yan S, Pan Y, Wang L, Liu J, Zhang Z, Huo W, Yang J, Huang Y (2017) Synthesis of low-cost porous ceramic microspheres from waste gangue for dye adsorption. J Adv Ceram 7(1):30–40

  38. Sadeghzadeh-Attar A (2020) Photocatalytic degradation evaluation of N-Fe codoped aligned TiO2 nanorods based on the effect of annealing temperature. J Adv Ceram 9(1):107–122

  39. Peng X, Li H, Shuai Q, Wang L (2020) Fire resistance of alkali activated geopolymer foams produced from metakaolin and Na2O2. Materials 13(3):535–542

    Article  CAS  Google Scholar 

  40. Yip CK, Lukey GC, Deventer J (2005) The coexistence of geopolymeric gel and calcium silicate hydrate at the early stage of alkaline activation. Cement Concrete Res 35(9):1688–1697

  41. Zheng X, Wu J (2021) Early strength development of soft clay stabilized by one-part ground granulated blast furnace slag and fly ash-based geopolymer. Front Mater 8:616430

  42. Bernal SA, Provis JL, Rose V, Mejía de Gutierrez R (2011) Evolution of binder structure in sodium silicate-activated slag-metakaolin blends. Cem Concr Compos 33(1):46–54

  43. Xiang J, Liu L, He Y, Zhang N, Cui X (2019) Early mechanical properties and microstructural evolution of slag/metakaolin-based geopolymers exposed to karst water. Cem Concr Compos 99:140–150

  44. Panda L, Rath SS, Rao DS, Nayak BB, Das B, Misra PK (2018) Thorough understanding of the kinetics and mechanism of heavy metal adsorption onto a pyrophyllite mine waste based geopolymer. J Mol Liq 263:428–441

  45. Yu Z, Lv X, Mao K, Yang A (2020) Role of in-situ formed free carbonon electromagnetic absorption properties of polymer-derived SiC ceramics. J Adv Ceram 9(5):617–628

  46. Chen P, Cao Z, Wen X, Wang J, Yang F, Qiu P, Yue Y, Liu G, Wang S, Zhong H (2017) A novel mesoporous silicate material (MS) preparation from dolomite and enhancing methylene blue removal by electronic induction. J Taiwan Inst Chem E 80:128–136

  47. Yan S, Zhang F, Kong J, Wang B, Li H, Yang Y, Xing P (2020) Mechanical properties of geopolymer composite foams reinforced with carbon nanofibers via modified hydrogen peroxide method. Mater Chem Phys 253:123258

  48. Siyal AA, Shamsuddin MR, Rabat NE, Zulfiqar M, Man Z, Low A (2019) Fly ash based geopolymer for the adsorption of anionic surfactant from aqueous solution. J Clean Prod 229:232–243

  49. Liu D, Ren X, Li Y, Tang Z, Zhang Z (2020) Nanowires-assembled WO3 nanomesh for fast detection of ppb-level NO2 at low temperature. J Adv Ceram 9(1):17–26

  50. Wu M, He Y, Wang L, Xia Q, Zhou A (2020) Synthesis and electrochemical propertied of V2C MXene by etching in opened/closed environments. J Adv Ceram 9(6):749–758

  51. Su Q, Yang S, He Y, Qin Z, Cui X (2020) Prepared self-growing supported nickel catalyst by recovering Ni(II) from metal wastewater using geopolymer microspheres. J Hazard Mater 389:121919

  52. Yu Z, Song W, Li J, Li Q (2020) Improved simultaneous adsorption of Cu(II) and Cr(VI) of organic modified metakaolin-based geopolymer. Arab J Chem 13(3):4811–4823

  53. Su Q, He Y, Yang S, Wan H, Chang S, Cui X (2021) Synthesis of NaA-zeolite microspheres by conversion of geopolymer and their performance of Pb (II) removal. Appl Clay Sci 200:105923

  54. Lertcumfu N, Jaita P, Thammarong S, Lamkhao S, Tandorn S, Randorn C, Tunkasiri T, Rujijanagul G (2020) Influence of graphene oxide additive on physical, microstructure, adsorption, and photocatalytic properties of calcined kaolinite-based geopolymer ceramic composites. Collold Surface A 602:125080

  55. Kara I, Tunc D, Sayin F, Akar ST (2018) Study on the performance of metakaolin based geopolymer for Mn(II) and Co(II) removal. Appl Clay Sci 161:184–193

  56. Lan T, Li P, Rehman FU, Li X, Yang W, Guo S (2019) Efficient adsorption of Cd2+ from aqueous solution using metakaolin geopolymers. Environ Sci Pollut Res Int 26(32):33555–33567

  57. Bhatti HN, Safa Y, Yakout SM, Shair OH, Iqbal M, Nazir A (2020) Efficient removal of dyes using carboxymethyl cellulose/alginate/polyvinyl alcohol/rice husk composite: Adsorption/desorption, kinetics and recycling studies. Int J Biol Macromol 150:861–870

  58. Wang L, Liu J, Rong Y, Yan S, Yu M, Li X, Wang Z, Zhang T, Yang J (2020) Novel design of microsphere adsorbent for efficient heavy metals adsorption. Int J Appl Ceram Tec 17(5):2228–2239

  59. Duan P, Yan C, Zhou W, Ren D (2016) Development of fly ash and iron ore tailing based porous geopolymer for removal of Cu(II) from wastewater. Ceram Int 42(12):13507–13518

  60. Al-Zboon K, Al-Harahsheh MS, Hani FB (2011) Fly ash-based geopolymer for Pb removal from aqueous solution. J Hazard Mater 188(1–3):414–421

  61. Abdelrahman EA, Abou El-Reash YG, Youssef HM, Kotp YH, Hegazey RM (2021) Utilization of rice husk and waste aluminum cans for the synthesis of some nanosized zeolite, zeolite/zeolite, and geopolymer/zeolite products for the efficient removal of Co(II), Cu(II), and Zn(II) ions from aqueous media. J Hazard Mater 401:123813

  62. Rossatto DL, Netto MS, Jahn SL, Mallmann ES, Dotto GL, Foletto EL (2020) Highly efficient adsorption performance of a novel magnetic geopolymer/Fe3O4 composite towards removal of aqueous acid green 16 dye. J Environ Chem Eng 8(3):103804

  63. Rożek P, Król M, Mozgawa W (2020) Lightweight geopolymer-expanded glass composites for removal of methylene blue from aqueous solutions. Ceram Int 46(12):19785

  64. Ma Z, Xue R, Li JS, Zhao Y, Chi SP (2021) Use of thermally modified waste concrete powder for removal of Pb (II) from wastewater: effects and mechanism. Environ Pollut 277:116776

  65. Yan C, Guo L, Ren D, Duan P (2019) Novel composites based on geopolymer for removal of Pb(II). Mater Lett 239:192–195

  66. Zhang J, Provis JL, Feng D, van Deventer JS (2008) Geopolymers for immobilization of Cr6+, Cd2+, and Pb2+ J Hazard Mater 157(2–3):587–598

  67. Yan S, Zhang F, Wang L, Rong Y, He P, Jia D, Yang J (2019) A green and low-cost hollow gangue microsphere/geopolymer adsorbent for the effective removal of heavy metals from wastewaters. J Environ Manage 246:174–183

  68. Tan TH, Mo KH, Ling TC, Lai SH (2020) Current development of geopolymer as alternative adsorbent for heavy metal removal. Environ Technol Inno 18:100684

  69. Qin L, Yan L, Chen J, Liu T, Yu H, Du B (2016) Enhanced removal of Pb2+, Cu2+, and Cd2+ by amino-functionalized magnetite/kaolin clay. Ind Eng Chem Res 55(27):7344–7354

  70. Wang Y, Han F, Mu J (2018) Solidification/stabilization mechanism of Pb(II), Cd(II), Mn(II) and Cr(III) in fly ash based geopolymers. Constr Build Mater 160:818–827

Download references

Acknowledgements

This project was supported by Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science (No. 2019JH3/30100016), Natural Science Foundation of Liaoning Province (No. 2019-BS-086), the Fundamental Research Funds for the Central Universities (No.N2025031).

Funding

This project was supported by Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science (No. 2019JH3/30100016), Natural Science Foundation of Liaoning Province (No. 2019-BS-086), the Fundamental Research Funds for the Central Universities (No.N2025031).

Author information

Authors and Affiliations

Authors

Contributions

All authors contributed to the study and design. Material preparation and data collection and analysis were done by Xue Feng. The Original draft was written by Xue Feng and Shu Yan, Writing and Review and Editing were done by Shengnan Jiang, Kai Huang, Xiaoqi Ren, Xinghong Du and Pengfei Xing. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Shu Yan.

Ethics declarations

Ethics Approval

Not applicable.

Consent to Participate

All the authors consent to participate.

Consent for Publication

All the authors give their consent for publication.

Competing Interests

The authors declare that they have no conflict of interest.

Conflict of Interest

The authors declare that they have no conflict of interest.

Disclosure of Potential Conflicts of Interest

The authors declare that they have no conflict of interest.

Research Involving Human Participants and/or Animals

Not applicable.

Informed Consent

Not applicable.

Additional information

Publisher’s Note

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

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Feng, X., Yan, S., Jiang, S. et al. Green Synthesis of the Metakaolin/slag Based Geopolymer for the Effective Removal of Methylene Blue and Pb (II). Silicon 14, 6965–6979 (2022). https://doi.org/10.1007/s12633-021-01439-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12633-021-01439-z

Keywords

Navigation