Skip to main content
SpringerLink
Log in

Synthesis and characterization of a cesium-selective macroporous silica-based supramolecular recognition material with high stability

  • Published:
Journal of Radioanalytical and Nuclear Chemistry Aims and scope Submit manuscript

Abstract

To design new and efficient supramolecular recognition material, a macroporous organic–inorganic bis(n-amyloxy)calix[4]arene-crown-6 (BnACalix[4]C6) material for separation of cesium from acidic solution was developed. The results of SEM, TG–DSC, FT-IR, 29Si NMR, and XRD characterizations indicated that BnACalix[4]C6 molecules were successfully impregnated into the pores of SiO2–P support. Cs(I) was shown to be both strongly and selectively adsorbed by this material at 3.0 M HNO3. The total organic carbon values showed that the leakage of BnACalix[4]C6 from BnACalix[4]C6/SiO2–P was below 0.1 %. Thus, BnACalix[4]C6/SiO2–P is a promising candidate for separation of Cs(I) from acidic HAW in SPEC process.

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

Similar content being viewed by others

References

  1. Gaur S (1996) Determination of Cs-137 in environmental water by ion-exchange chromatography. J Chromatogr A 733:57–71

    Article  CAS  Google Scholar 

  2. Todd TA, Brewer KN, Wood DJ, Tullock PA, Mann NR, Olson LG (2001) Evaluation and testing of inorganic ion exchange sorbents for the removal of 137Cs from actual Idaho nuclear technology and engineering center acidic tank waste. Sep Sci Technol 36:999–1016

    Article  CAS  Google Scholar 

  3. Dozol JF, Dozol M, Macias RM (2000) Extraction of strontium and cesium by dicarbollides, crown ethers and functionalized calixarenes. J Incl Phenom Macrocycl Chem 38:1–22

    Article  CAS  Google Scholar 

  4. Aghayan H, Mahjoub AR, Khanchi AR (2012) Immobilization of Tin (IV) molybdophosphate onto mesoporous silica SBA-15 and its application on strontium removal from aqueous solution. Appl Surf Sci 261:14–20

    Article  CAS  Google Scholar 

  5. Aghayan H, Khanchi AR, Mahjoub AR (2013) Synthesis and characterization of cesium molybdo vanado phosphate immobilized on platelet SBA-15: an efficient inorganic composite ion-exchanger for gadolinium ion sorption. Appl Surf Sci 274:7–14

    Article  CAS  Google Scholar 

  6. Suzuki N, Ozawa S, Ochi K, Chikuma T, Watanabe Y (2013) Approaches for cesium uptake by vermiculite. J Chem Technol Biotechnol 88:1603–1605

    Article  CAS  Google Scholar 

  7. Riddle CL, Baker JD, Law JD, McGrath CA, Meikrantz DH, Mincher BJ, Peterman DR, Todd TA (2005) Fission product extraction FPEX): development of a novel solvent for the simultaneous separation of strontium and cesium from acidic solutions. Solvent Extr Ion Exch 23:449–461

    Article  CAS  Google Scholar 

  8. Walker DD, Norato MA, Campbell SG, Crowder ML, Fink SD, Fondeur FF, Geeting MW, Kessinger GF, Pierce RA (2005) Cesium removal from Savannah River site radioactive waste using the caustic-side solvent extraction (CSSX) process. Sep Sci Technol 40:297–309

    Article  CAS  Google Scholar 

  9. Bazelaire E, Gorbunova MG, Bonnesen PV, Moyer BA, Delmau LH (2004) PH-Switchable cesium nitrate extraction with calix[4]arene mono and bis(benzo-crown-6) ethers bearing amino functionalities. Solvent Extr Ion Exch 22:637–661

    Article  CAS  Google Scholar 

  10. Tel H, Altas Y, Gur F, Ugur A (2010) Sorption kinetics of cesium on ZrO2 and ZrO2–SiO2–TiO2 microspheres. Radiochim Acta 98:215–219

    Article  CAS  Google Scholar 

  11. El-Kamash AM (2008) Evaluation of zeolite A for the sorptive removal of Cs+ and Sr2+ ions from aqueous solutions using batch and fixed bed column operations. J Hazard Mater 151:432–445

    Article  CAS  Google Scholar 

  12. Endo M, Yoshikawa E, Muramatsu N, Takizawa N, Kawai T, Unuma H, Sasaki A, Masano A, Takeyama Y, Kahara T (2013) The removal of cesium ion with natural Itaya zeolite and the ion exchange characteristics. J Chem Technol Biotechnol 88:1597–1602

    Article  CAS  Google Scholar 

  13. Haas PA (1993) A review of information on ferrocyanide solids for removal of cesium from solutions. Sep Sci Technol 28:2479–2506

    Article  CAS  Google Scholar 

  14. Murthy GS, Sivaiah MV, Kumar SS, Reddy VN, Krishna RM, Lakshminarayana S (2004) Adsorption of cesium on a composite inorganic exchanger zirconium phosphate–ammonium molybdophosphate. J Radioanal Nucl Chem 260:109–114

    Article  CAS  Google Scholar 

  15. Abd El-Latif MM, Elkady MF (2010) Equilibrium isotherms for harmful ions sorption using nano zirconium vanadate ion exchanger. Desalination 255:21–43

    Article  CAS  Google Scholar 

  16. El-Latif MMA, Elkady MF (2011) Kinetics study and thermodynamic behavior for removing cesium, cobalt and nickel ions from aqueous solution using nano-zirconium vanadate ion exchanger. Desalination 271:41–54

    Article  CAS  Google Scholar 

  17. Moller T, Harjula R (2001) Uptake of various radionuclides by hydrothermally prepared molybdenum phosphates. Sep Sci Technol 36:885–897

    Article  CAS  Google Scholar 

  18. Peterskova M, Valderrama C, Gibert O, Cortina JL (2012) Extraction of valuable metal ions (Cs, Rb, Li, U) from reverse osmosis concentrate using selective sorbents. Desalination 286:316–323

    Article  CAS  Google Scholar 

  19. Yu B, Chen J, Song CL (2002) Crystalline silicotitanate: a new type of ion exchanger for Cs removal from liquid waste. J Mater Sci Technol 18:206–210

    CAS  Google Scholar 

  20. Popa K, Pavel CC (2012) Radioactive wastewaters purification using titanosilicates materials: state of the art and perspectives. Desalination 293:78–86

    Article  CAS  Google Scholar 

  21. Fiskum SK, Blanchard DL, Steele MJ, Thomas KK, Trang-Le T, Thorson MR (2006) Spherical resorcinol-formaldehyde resin testing for cesium removal from Hanford tank waste simulant. Sep Sci Technol 41:2461–2474

    Article  CAS  Google Scholar 

  22. Manos MJ, Ding N, Kanatzidis MG (2008) Layered metal sulfides: exceptionally selective agents for radioactive strontium removal. Proc Natl Acad Sci USA 105:3696–3699

    Article  Google Scholar 

  23. Manos MJ, Kanatzidis MG (2009) Highly efficient and rapid Cs+ uptake by the layered metal sulfide K2xMnxSn3-xS6 (KMS-1). J Am Chem Soc 131:6599–6607

    Article  CAS  Google Scholar 

  24. Arena G, Casnati A, Contino A, Mirone L, Sciotto D, Ungaro R (1996) Synthesis of new calixcrowns and their anchoring to silica gel for the selective separation of Cs+ and K+. Chem Commun 19:2277–2278

    Article  Google Scholar 

  25. Dietz ML, Ensor DD, Harmon B, Seekamp S (2006) Separation and preconcentration of cesium from acidic media by extraction chromatography. Sep Sci Technol 41:2183–2204

    Article  CAS  Google Scholar 

  26. Xiao CL, Zhang AY, Chai ZF (2012) Synthesis and characterization of a new polymer-based supramolecular recognition material and its adsorption for cesium. Solvent Extr Ion Exch 30:17–32

    Article  CAS  Google Scholar 

  27. Zhang AY, Xiao CL, Kuraoka E, Kumagai M (2007) Preparation of a novel silica-based DtBuCH18C6 impregnated polymeric composite modified by tri-n-butyl phosphate and its application in chromatographic partitioning of strontium from high level liquid waste. Ind Eng Chem Res 46:2164–2171

    Article  CAS  Google Scholar 

  28. Zhang AY, Hu QH, Chai ZF (2009) SPEC: a new process for strontium and cesium partitioning utilizing two macroporous silica-based supramolecular recognition agents impregnated polymeric composites. Sep Sci Technol 44:2146–2168

    Article  CAS  Google Scholar 

  29. Zhang AY, Xiao CL, Chai ZF (2009) SPEC process II. Adsorption of strontium and some typical co-existent elements contained in high level liquid waste onto a macroporous silica-based crown ether impregnated functional composite. J Radioanal Nucl Chem 280:181–191

    Article  CAS  Google Scholar 

  30. Zhang AY, Chen CM, Chat ZF, Kumagai M (2008) SPEC process III. Synthesis of a macroporous silica-based crown ether-impregnated polymeric composite modified with 1-octanol and its adsorption capacity for Sr(II) ions and some typical co-existent metal ions. Adsorpt Sci Technol 26:705–720

    Article  CAS  Google Scholar 

  31. Xiao CL, Zhang AY, Chai ZF (2014) Synthesis and characterization of a novel organic-inorganic hybrid supramolecular recognition material and its selective adsorption for cesium. J Radioanal Nucl Chem 299:699–708

    Article  CAS  Google Scholar 

  32. Zhang AY, Chai ZF (2012) Adsorption property of cesium onto modified macroporous silica-calix[4]arene-crown based supramolecular recognition materials. Ind Eng Chem Res 51:6196–6204

    Article  CAS  Google Scholar 

  33. Casnati A, Pochini A, Ungaro R, Ugozzoli F, Arnaud F, Fanni S, Schwing MJ, Egberink RJM, Dejong F, Reinhoudt DN (1995) Synthesis, complexation, and membrane-transport studies of 1,3-alternate calix[4]arene-crown-6 conformers—a new class of cesium selective ionophores. J Am Chem Soc 117:2767–2777

    Article  CAS  Google Scholar 

  34. Zhang AY, Wei YZ, Kumagai M (2004) Synthesis of a novel macroporous silica-based polymeric material containing 4,4’, (5’)-di(tert-butylcyclohexano)18-crown-6 functional group and its adsorption mechanism for strontium. React Funct Polym 61:191–202

    Article  CAS  Google Scholar 

  35. Zhang AY, Xiao CL, Liu YH, Hu QH, Chen CM, Kuraoka E (2010) Preparation of macroporous silica-based crown ether materials for strontium separation. J Porous Mater 17:153–161

    Article  CAS  Google Scholar 

  36. Ungaro R, Casnati A, Ugozzoli F, Pochini A, Dozol JF, Hill C, Rouquette H (1994) 1,3-Dialkoxycalix[4]arenecrowns-6 in 1,3-alternate conformation—cesium-selective ligands that exploit cation-arene interactions. Angew Chem Int Ed 33:1506–1509

    Article  Google Scholar 

  37. Asfari Z, Bressot C, Vicens J, Hill C, Dozol JF, Rouquette H, Eymard S, Lamare V, Tournois B (1995) Doubly crowned calix[4]arenes in the 1,3-alternate conformation as cesium-selective carriers in supported liquid membranes. Anal Chem 67:3133–3139

    Article  CAS  Google Scholar 

  38. Kim JS, Pang JH, Yu IY, Lee WK, Suh IH, Kim JK, Cho MH, Kim ET, Ra DY (1999) Calix[4]arene dibenzocrown ethers as caesium selective extractants. J Chem Soc Perkin Trans 2:837–846

    Article  Google Scholar 

  39. Casnati A, Sansone F, Dozol JF, Rouquette H, Arnaud-Neu F, Byrne D, Fuangswasdi S, Schwing-Weill MJ, Ungaro R (2001) New calix[4]arene-monobenzo- and -dibenzo-crown-6 as cesium selective ionophores in the radioactive waste treatment: synthesis, complexation and extraction properties. J Incl Phenom Macrocycl Chem 41:193–200

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This work was financially supported by the National Natural Science Foundation of China under contracts No. 20671081 and No. 91126021, Zhejiang Provincial Natural Science Foundation of China under contract No. Y4110002, Zhejiang Provincial Commonweal Technology Applied Research Project under contract No. 2012C23032, and a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

Author information

Authors and Affiliations

  1. School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University, 199 Ren’ai Road, Suzhou, 215123, People’s Republic of China

    Chengliang Xiao

  2. Department of Chemical and Biochemical Engineering, Zhejiang University, 38 Zheda Road, Hangzhou, 310027, People’s Republic of China

    Anyun Zhang

  3. Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, 199 Ren’ai Road, Suzhou, 215123, People’s Republic of China

    Chengliang Xiao

Authors
  1. Chengliang Xiao
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Anyun Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Chengliang Xiao or Anyun Zhang.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Xiao, C., Zhang, A. Synthesis and characterization of a cesium-selective macroporous silica-based supramolecular recognition material with high stability. J Radioanal Nucl Chem 307, 713–723 (2016). https://doi.org/10.1007/s10967-015-4171-9

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-015-4171-9

Keywords

Search

Navigation