Skip to main content
SpringerLink
Log in

Synthesis of bi-functional chelating sorbent for recovery of uranium from aqueous solution: sorption, kinetics and reusability studies

  • Original Paper
  • Published:
Journal of Polymer Research Aims and scope Submit manuscript

Abstract

A bi-functional chelating sorbent is synthesised by introducing two different functionalities (amine and amidoxime groups) subsequently on the surface of an earlier synthesized cross-linked poly-acrylonitrile beads. The cross-linked base polymer beads are normally synthesised through suspension polymerisation using acrylonitrile and styrene as monomers and divinyl benzene as cross-linking agent. The bi-functionality is introduced by amination of base polymer in the first step by reacting with diethylenetriamine followed by amidoximation reaction with hydroxylamine hydrochloride in the second step. The incorporation of functional groups on beads are identified and confirmed with FTIR spectroscopy while the surface morphology, porosity and pores dimensions are evaluated by SEM and BET techniques. The saturation sorption capacity of synthesized beads for uranyl ion is tested and found ~ 45 mg g−1, which is significantly higher than the beads functionalized with sole amidoxime group. These bi-functional beads are quite efficient over a wide pH (1–10) range. The kinetics measurements indicate that the synthesized sorbents reach its saturation sorption capacity within 2 h at ~25 °C under neutral pH. In this study, the sorbed uranyl ions are eluted out with 1 M HCl efficiently. These beads exhibit excellent reusability up to three cycles without losing much of its capacity, suggesting better usability in real samples.

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
Scheme 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Scheme 2
Scheme 3
Fig. 8

Similar content being viewed by others

References

  1. Seko N, Katakai A, Tamada M, Sugo T, Yoshii F (2004) Fine fibrous amidoxime adsorbent synthesized by grafting and uranium adsorption-elution cyclic test with seawater. Sep Sci Technol 39:3753–3767

    CAS  Google Scholar 

  2. Benedict B, Pigford TH, Lewi HW (1981) Nuclear Chemical Engineering. McGraw-Hill

    Google Scholar 

  3. Gadd GM (2000) Bioremedial potential of microbial mechanisms of metal mobilization and immobilization. Curr Opin Biotechnol 11:271–279

    CAS  PubMed  Google Scholar 

  4. Egawa H, Kabay N, Shuto T, Jyo A (2003) Recovery of uranium from seawater. XII. Preparation and characterization of lightly crosslinked highly porous chelating resins containing amidoxime groups. J Appl Polym Sci 46:129–142

    Google Scholar 

  5. Kabay N, Egawa H (1994) Chelating polymers for recovery of uranium from seawater. Sep Sci Technol 29:135–150

    CAS  Google Scholar 

  6. Chmielewski AG, Urbański TS, Migdał W (1997) Separation technologies for metals recovery from industrial wastes. Hydrometallurgy 45:333–344

    CAS  Google Scholar 

  7. Ritcey GM (1980) Crud in solvent extraction processing — a review of causes and treatment. Hydrometallurgy 5:97–107

    CAS  Google Scholar 

  8. Hudson MJ (1982) An introduction to some aspects of solvent extraction chemistry in hydrometallurgy. Hydrometallurgy 9:149–168

    CAS  Google Scholar 

  9. Hoh Y-C, Chuang W-Y, Wang W-K (1986) Interfacial tension studies on the extraction of lanthanum by D2EHPA. Hydrometallurgy 15:381–390

    CAS  Google Scholar 

  10. Tripathi SC, Bindu P, Ramanujam A (2001) Studies on the identification of harmful radiolytic products of 30% TBP-n-dodecane-HNO3 by gas liquid chromatography. i. formation of diluent degradation products and their role in Pu retention behavior. Sep Sci Technol 36:1463–1478

    CAS  Google Scholar 

  11. Bae SY, Southard GL, Murray GM (1999) Molecularly imprinted ion exchange resin for purification, preconcentration and determination of UO22+by spectrophotometry and plasma spectrometry. Anal Chim Acta 397:173–181

    CAS  Google Scholar 

  12. Seyhan S, Merdivan M, Demirel N (2008) Use of o-phenylene dioxydiacetic acid impregnated in Amberlite XAD resin for separation and preconcentration of uranium(VI) and thorium(IV). J Hazard Mater 152:79–84

    CAS  PubMed  Google Scholar 

  13. Sadeghi S, Sheikhzadeh E (2009) Solid phase extraction using silica gel modified with murexide for preconcentration of uranium (VI) ions from water samples. J Hazard Mater 163:861–868

    CAS  PubMed  Google Scholar 

  14. Northcott SE, Leyden DE (1981) Separation of uranium from molybdenum using a diamine functional group bonded to controlled-pore glass. Anal Chim Acta 126:117–124

    CAS  Google Scholar 

  15. Girgin S, Acarkan N, Sirkeci AA (2002) The uranium(VI) extraction mechanism of D2EHPA-TOPO from a wet process phosphoric acid. J Radioanal Nucl Chem 251:263–271

    CAS  Google Scholar 

  16. Singh Krishan K, Pathak Sanjay K, Kumar M, Mahtele AK, Tripathi SC, Bajaj Parma N (2013) Study of uranium sorption using D2EHPA-impregnated polymeric beads. J Appl Polym Sci 130:3355–3364

    Google Scholar 

  17. Singh K, Shah C, Dwivedi C, Kumar M, Bajaj Parma N (2012) Study of uranium adsorption using amidoximated polyacrylonitrile-encapsulated macroporous beads. J Appl Polym Sci 127:410–419

    Google Scholar 

  18. Toker Y, Eral M, Hicsonmez U (1998) Recovery of uranium from aqueous solutions by trioctylamine impregnated polyurethane foam. Analyst 123:51–53

    CAS  Google Scholar 

  19. Huang G, Li W, Liu Q, Liu J, Zhang H, Li R, Li Z, Jing X, Wang J (2018) Efficient removal of uranium (VI) from simulated seawater with hyperbranched polyethylenimine (HPEI)-functionalized polyacrylonitrile fibers, New. J Chem 42:168–176

    CAS  Google Scholar 

  20. Sebesta F, John J, Motl A (1997) Development of composite ion exchangers and their use in treatment of liquid radioactive wastes. International Atomic Energy Agency (IAEA) pp 79–103

  21. Omichi H, Katakai A, Sugo T, Okamoto J (1986) A new type of amidoxime-group-containing adsorbent for the recovery of uranium from seawater. II. Effect of grafting of hydrophilic monomers. Sep Sci Technol 21:299–313

    CAS  Google Scholar 

  22. Kabay N, Katakai A, Sugo T, Egawa H (2003) Preparation of fibrous adsorbents containing amidoxime groups by radiation-induced grafting and application to uranium recovery from sea water. J Appl Polym Sci 49:599–607

    Google Scholar 

  23. Prasad TL, Saxena AK, Tewari PK, Sathiyamoorthy D (2009) An engineering scale study on radiation grafting of polymeric adsorbents for recovery of heavy metal ions from seawater. Nucl Eng Technol 41:1101–1108

    CAS  Google Scholar 

  24. Şahiner N, Pekel N, Güven O (1999) Radiation synthesis, characterization and amidoximation of N-vinyl-2-pyrrolidone/acrylonitrile interpenetrating polymer networks. React Funct Polym 39:139–146

    Google Scholar 

  25. Arica MY, Bayramoglu G (2016) Polyaniline coated magnetic carboxymethylcellulose beads for selective removal of uranium ions from aqueous solution. J Radioanal Nucl Chem 310:711–724

    CAS  Google Scholar 

  26. Bayramoglu G, Arica MY (2016) MCM-41 silica particles grafted with polyacrylonitrile: Modification in to amidoxime and carboxyl groups for enhanced uranium removal from aqueous medium. Microporous Mesoporous Mater 226:117–124

    CAS  Google Scholar 

  27. Bayramoglu G, Yakup Arica M (2016) Amidoxime functionalized Trametes trogii pellets for removal of uranium(VI) from aqueous medium. J Radioanal Nucl Chem 307:373–384

    CAS  Google Scholar 

  28. Bayramoglu G, Akbulut A, Arica MY (2015) Study of polyethyleneimine- and amidoxime-functionalized hybrid biomass of Spirulina (Arthrospira) platensis for adsorption of uranium (VI) ion. Environ Sci Pollut Res 22:17998–18010

    CAS  Google Scholar 

  29. Bayramoglu G, Akbulut A, Acıkgoz-Erkaya I, Arica MY (2018) Uranium sorption by native and nitrilotriacetate-modified Bangia atropurpurea biomass: kinetics and thermodynamics. J Appl Phycol 30:649–661

    CAS  Google Scholar 

  30. Chi F, Zhang S, Wen J, Xiong J, Hu S (2018) Highly efficient recovery of uranium from seawater using an electrochemical approach. Ind Eng Chem Res 57:8078–8084

    CAS  Google Scholar 

  31. Alexandratos SD, Zhu X, Florent M, Sellin R (2016) Polymer-supported bifunctional amidoximes for the sorption of uranium from seawater. Ind Eng Chem Res 55:4208–4216

    CAS  Google Scholar 

  32. Abney CW, Mayes RT, Saito T, Dai S (2017) Materials for the recovery of uranium from seawater. Chem Rev 117:13935–14013

    CAS  PubMed  Google Scholar 

  33. Kanjilal A, Singh KK, Bairwa KK, Kumar M (2019) Synthesis and study of optimization of amidoximated PAN-DVB-EGDMA beads for the sorption of uranium from aqueous media. Polym Eng Sci 59:863–872

    CAS  Google Scholar 

  34. Bahramifar N, Yamini Y (2005) On-line preconcentration of some rare earth elements in water samples using C18-cartridge modified with l-(2-pyridylazo) 2-naphtol (PAN) prior to simultaneous determination by inductively coupled plasma optical emission spectrometry (ICP–OES). Anal Chim Acta 540:325–332

    CAS  Google Scholar 

  35. Scott RH, Strasheim A, Kokot ML (1976) The determination of uranium in rocks by inductively coupled plasma-optical emission spectrometry. Anal Chim Acta 82:67–77

    CAS  Google Scholar 

  36. Santos JS, Teixeira LSG, dos Santos WNL, Lemos VA, Godoy JM, Ferreira SLC (2010) Uranium determination using atomic spectrometric techniques: An overview. Anal Chim Acta 674:143–156

    CAS  PubMed  Google Scholar 

  37. Shao D, Hou G, Chi F, Lu X, Ren X (2021) Transformation details of poly(acrylonitrile) to poly(amidoxime) during the amidoximation process. RSC Adv 11:1909–1915

    CAS  Google Scholar 

  38. Brandani S (2021) Kinetics of liquid phase batch adsorption experiments. Adsorption 27:353–368

    CAS  Google Scholar 

  39. Hubbe MA, Azizian S, Douven S (2019) Implications of apparent pseudo-second-order adsorption kinetics onto cellulosic materials: A review. BioResources 14:7582–7626

    Google Scholar 

  40. Hubbe MA (2021) Insisting upon meaningful results from adsorption experiments. Sep Purif Rev. https://doi.org/10.1080/15422119.2021.1888299

    Article  Google Scholar 

  41. Tran HN, You SJ, Hosseini-Bandegharaei A, Chao HP (2017) Mistakes and inconsistencies regarding adsorption of contaminants from aqueous solutions: A critical review. Water Res 120:88–116

    CAS  PubMed  Google Scholar 

  42. Ho Y, McKay G (1998) A comparison of chemisorption kinetic models applied to pollutant removal on various sorbents, Process Saf. Environ Prot 76:332–340

    CAS  Google Scholar 

  43. Yang X, Al-Duri B (2005) Kinetic modeling of liquid-phase adsorption of reactive dyes on activated carbon. J Colloid Interface Sci 287:25–34

    CAS  PubMed  Google Scholar 

  44. Boyd GE, Adamson AW, Myers LS (1947) The exchange adsorption of ions from aqueous solutions by organic zeolites. II. Kinetics1. J Am Chem Soc 69:2836–2848

    CAS  PubMed  Google Scholar 

  45. Langmuir I (1918) The adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40:1361–1403

    CAS  Google Scholar 

  46. Freundlich HMFZ (1906) Over the adsorption in solution. J Phys Chem 57:385–471

    CAS  Google Scholar 

  47. Allen SJ, Gan Q, Matthews R, Johnson PA (2003) Comparison of optimised isotherm models for basic dye adsorption by kudzu. Bioresour Technol 88:143–152

    CAS  PubMed  Google Scholar 

  48. Vukovic S, Watson LA, Kang SO, Custelcean R, Hay BP (2012) How amidoximate binds the uranyl cation. Inorg Chem 51:3855–3859

    CAS  PubMed  Google Scholar 

  49. Mehio N, Lashely MA, Nugent JW, Tucker L, Correia B, Do-Thanh C-L, Dai S, Hancock RD, Bryantsev VS (2015) Acidity of the amidoxime functional group in aqueous solution: A combined experimental and computational study. J Phys Chem B 119:3567–3576

    CAS  PubMed  Google Scholar 

  50. Greenwood NNEA (1997) Chemistry of the Elements, Second, Butterworth-Heineman, Oxford

  51. Piron E, Domard A (1998) Interaction between chitosan and uranyl ions. Part 2. Mechanism of interaction, Int J Biol Macromol 22:33–40

    CAS  Google Scholar 

  52. Tang N, Liang J, Niu C, Wang H, Luo Y, Xing W, Ye S, Liang C, Guo H, Guo J, Zhang Y, Zeng G (2020) Amidoxime-based materials for uranium recovery and removal. J Mater Chem A 8:7588–7625

    CAS  Google Scholar 

  53. Humelnicu D, Dinu MV, Drăgan ES (2011) Adsorption characteristics of UO22+ and Th4+ ions from simulated radioactive solutions onto chitosan/clinoptilolite sorbents. J Hazard Mater 185:447–455

    CAS  PubMed  Google Scholar 

  54. Ramachandhran V, Kumar SC, Sudarsanan M (2001) Preparation, characterization, and performance evaluation of styrene-acrylonitrile-amidoxime sorbent for uranium recovery from dilute solutions. J Macromol Sci A 38:1151–1166

    Google Scholar 

  55. Pal S, Ramachandhran V, Prabhakar S, Tewari PK, Sudersanan M (2006) Polyhydroxamic acid sorbents for uranium recovery. J Macromol Sci A 43:735–747

    CAS  Google Scholar 

  56. Chauhan GS, Kumar A (2008) A study in the uranyl ions uptake on acrylic acid and acrylamide copolymeric hydrogels. J Appl Polym Sci 110:3795–3803

    CAS  Google Scholar 

  57. Zhang H, Liang H, Chen Q, Shen X (2013) Synthesis of a new ionic imprinted polymer for the extraction of uranium from seawater. J Radioanal Nucl Chem 298:1705–1712

    CAS  Google Scholar 

Download references

Acknowledgements

This research was carried out under the plan project no: RBA4013. Authors thank the Department of Atomic Energy, Government of India and Bhabha Atomic Research Centre for funding and all the members of Radiation and Photochemistry Division for their support.

Author information

Authors and Affiliations

  1. Radiation and Photochemistry Division, Bhabha Atomic Research Centre, Trombay, Mumbai, 400085, India

    Amit Kanjilal, Krishan Kant Singh & G. R. Dey

  2. Homi Bhabha National Institute, Anushaktinagar, Mumbai, 400094, India

    Krishan Kant Singh, A. K. Tyagi & G. R. Dey

  3. Chemistry Group, Bhabha Atomic Research Centre, Trombay, Mumbai, 400085, India

    A. K. Tyagi

Authors
  1. Amit Kanjilal
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Krishan Kant Singh
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. A. K. Tyagi
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. G. R. Dey
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to G. R. Dey.

Ethics declarations

Conflict of interest

No conflict.

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

Kanjilal, A., Singh, K.K., Tyagi, A.K. et al. Synthesis of bi-functional chelating sorbent for recovery of uranium from aqueous solution: sorption, kinetics and reusability studies. J Polym Res 28, 460 (2021). https://doi.org/10.1007/s10965-021-02819-0

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s10965-021-02819-0

Keywords

Search

Navigation