Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture

Hyungmin Jeon, Susung Lee, Jeong-Chul Kim, Minkee Choi

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Front. Chem. Sci. Eng. ›› 2024, Vol. 18 ›› Issue (9) : 98. DOI: 10.1007/s11705-024-2449-6
RESEARCH ARTICLE

Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture

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Abstract

NaA zeolite (Si/Al = 1.00) has been commercially applied for capturing radioactive 90Sr2+ because of its high surface charge density, effectively stabilizing the multivalent cation. However, owing to its narrow micropore opening (4.0 Å), large micron-sized crystallites, and bulkiness of hydrated Sr2+, the Sr2+ exchange over NaA has been limited by very slow kinetics. In this study, we synthesized nanocrystalline low-silica X by minimizing a water content in a synthesis gel and utilizing a methyl cellulose hydrogel as a crystal growth inhibitor. The resulting zeolite exhibited high crystallinity and Al-rich framework (Si/Al of approximately 1.00) with the sole presence of tetrahedral Al sites, which are capable of high Sr2+ uptake and ion selectivity. Meanwhile, the zeolite with a FAU topology has a much larger micropore opening size (7.4 Å) and a much smaller crystallite size (~340 nm) than NaA, which enable significantly enhanced ion-exchange kinetics. Compared to conventional NaA, the nanocrystalline low-silica X exhibited remarkably increased Sr2+-exchange kinetics (> 18-fold larger rate constant) in batch experiments. Although both the nanocrystalline low-silica X and NaA exhibited comparable Sr2+ capacities under equilibrated conditions, the former demonstrated a 5.5-fold larger breakthrough volume than NaA under dynamic conditions, attributed to its significantly faster Sr2+-exchange kinetics.

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Keywords

Sr2+ removal / low-silica X zeolite / nanocrystal / hydrogel / methyl cellulose

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Hyungmin Jeon, Susung Lee, Jeong-Chul Kim, Minkee Choi. Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture. Front. Chem. Sci. Eng., 2024, 18(9): 98 https://doi.org/10.1007/s11705-024-2449-6

References

[1]
Zhang Z , Cheng M , Xiao X , Bi K , Song T , Hu K Q , Dai Y , Zhou L , Liu C , Ji X . . Machine-learning-guided identification of coordination polymer ligands for crystallizing separation of Cs/Sr. ACS Applied Materials & Interfaces, 2022, 14(29): 33076–33084
CrossRef Google scholar
[2]
Delacroix D , Guerre J P , Leblanc P , Hickman C . Radionuclide and radiation protection data handbook 2002. Radiation Protection Dosimetry, 2022, 98(1): 1–168
CrossRef Google scholar
[3]
Avery S V . Caesium accumulation by microorganisms: uptake mechanism, cation competition, compartmentalization and toxicity. Journal of Industrial Microbiology, 1995, 14(2): 76–84
CrossRef Google scholar
[4]
GuptaD KWaltherC. Behaviour of strontium in plants and the environment. 2018, Springer, Cham
[5]
El-Rahman K M A , El-Kamash A M , El-Sourougy M R , Abdel-Moniem N M . Thermodynamic modeling for the removal of Cs+, Sr2+, Ca2+ and Mg2+ ions from aqueous waste solutions using zeolite A. Journal of Radioanalytical and Nuclear Chemistry, 2006, 268(2): 221–230
CrossRef Google scholar
[6]
Han E , Kim Y G , Yang H M , Yoon I H , Choi M . Synergy between zeolite framework and encapsulated sulfur for enhanced ion-exchange selectivity to radioactive cesium. Chemistry of Materials, 2018, 30(16): 5777–5785
CrossRef Google scholar
[7]
Kwon S , Kim C , Han E , Lee H , Cho H S , Choi M . Relationship between zeolite structure and capture capability for radioactive cesium and strontium. Journal of Hazardous Materials, 2021, 408: 124419
CrossRef Google scholar
[8]
Zhang X , Liu Y . Ultrafast removal of radioactive strontium ions from contaminated water by nanostructured layered sodium vanadosilicate with high adsorption capacity and selectivity. Journal of Hazardous Materials, 2020, 398: 122907
CrossRef Google scholar
[9]
Zhang H , Li C , Chen X , Fu H , Chen Y , Ning S , Fujita T , Wei Y , Wang X . Layered ammonium vanadate nanobelt as efficient adsorbents for removal of Sr2+ and Cs+ from contaminated water. Journal of Colloid and Interface Science, 2022, 615: 110–123
CrossRef Google scholar
[10]
Anthony R G , Philip C V , Dosch R G . Selective adsorption and ion exchange of metal cations and anions with silico-titanates and layered titanates. Waste Management, 1993, 13(5–7): 503–512
CrossRef Google scholar
[11]
Chitra S , Viswanathan S , Rao S V S , Sinha P K . Uptake of cesium and strontium by crystalline silicotitanates from radioactive wastes. Journal of Radioanalytical and Nuclear Chemistry, 2011, 287(3): 955–960
CrossRef Google scholar
[12]
Wang S , Ning S , Zhang W , Zhang S , Zhou J , Wang X , Wei Y . Synthesis of carboxyl group functionalized silica composite resin for strontium removal. Materials & Design, 2020, 185: 108224
CrossRef Google scholar
[13]
Manos M J , Ding N , Kanatzidis M G . Layered metal sulfides: exceptionally selective agents for radioactive strontium removal. Proceedings of the National Academy of Sciences of the United States of America, 2008, 105(10): 3696–3699
CrossRef Google scholar
[14]
Schneider S , Garcez A C , Tremblay M , Bilodeau F , Lariviere D , Kleitz F . Nanoporous ammonium molybdophosphate-silica hybrids as regenerable ultra-selective extraction agents for radiocesium monitoring. New Journal of Chemistry, 2013, 37(12): 3877–3880
CrossRef Google scholar
[15]
Jeon H , Seok J , Ha Y , Kim J C , Cho H S , Yang H M , Choi M . First successful synthesis of an Al-rich mesoporous aluminosilicate for fast radioactive strontium capture. Journal of Hazardous Materials, 2023, 451: 131136
CrossRef Google scholar
[16]
Zhang J , Chen L , Gui D , Zhang H , Zhang D , Liu W , Huang G , Diwu J , Chai Z , Wang S . . An ingenious one-dimensional zirconium phosphonate with efficient strontium exchange capability and moderate proton conductivity. Dalton Transactions, 2018, 47(15): 5161–5165
CrossRef Google scholar
[17]
Zhang J , Chen L , Dai X , Chen L , Zhai F , Yu W , Guo S , Yang L , Chen L , Zhang Y . . Efficient Sr-90 removal from highly alkaline solution by an ultrastable crystalline zirconium phosphonate. Chemical Communications, 2021, 57(68): 8452–8455
CrossRef Google scholar
[18]
Tang X , Wang S , Zhang Z , Li Z , Wang L , Yuan L , Wang B , Sun J , Zheng L , Wang H . . Graphene oxide/chitosan/potassium copper hexacyanoferrate(II) composite aerogel for efficient removal of cesium. Chemical Engineering Journal, 2022, 444: 136397
CrossRef Google scholar
[19]
Vashnia S , Tavakoli H , Cheraghali R , Sepehrian H . Supporting of lead hexacyanoferrate on mesoporous MCM-41 and its use as effective adsorbent for strontium: equilibrium, kinetic, and thermodynamic studies. Separation Science and Technology, 2014, 49(2): 241–248
CrossRef Google scholar
[20]
McAleer A M , Rees L V C , Nowak A K . Ion exchange and aluminum distribution in ZSM-5 zeolites. Zeolites, 1991, 11(4): 329–336
CrossRef Google scholar
[21]
Watling T C , Rees L V C . Ion exchange in zeolite EU-1: Part 1. The effect of Si/Al ratio. Zeolites, 1994, 14(8): 687–692
CrossRef Google scholar
[22]
Hassan H S , Moamen O A A , Zaher W F . Adaptive neuro-fuzzy inference system analysis on sorption studies of strontium and cesium cations onto a novel impregnated nano-zeolite. Advanced Powder Technology, 2020, 31(3): 1125–1139
CrossRef Google scholar
[23]
Barrer R M , Bartholomew R F , Rees L V C . Ion exchange in porous crystals, Part I. self- and exchange-diffusion of ions in chabazites. Journal of Physics and Chemistry of Solids, 1963, 24(1): 51–62
CrossRef Google scholar
[24]
El-Kamash A M . Evaluation of zeolite A for the sorptive removal of Cs+ and Sr2+ ions from aqueous solutions using batch and fixed bed column operation. Journal of Hazardous Materials, 2008, 151(2-3): 432–445
CrossRef Google scholar
[25]
Merceille A , Weinzaepfel E , Barré Y , Grandjean A . The sorption behaviour of synthetic sodium nonatitanate and zeolite A for removing radioactive strontium from aqueous wastes. Separation and Purification Technology, 2012, 96: 81–88
CrossRef Google scholar
[26]
Mimura H , Kanno T . Distribution and fixation of cesium and strontium in zeolite A and chabazite. Journal of Nuclear Science and Technology, 1985, 22(4): 284–291
CrossRef Google scholar
[27]
Said B , Grandjean A , Barre Y , Tancret F , Fajula F , Galarneau A . LTA zeolite monoliths with hierarchical trimodal porosity as highly efficient microreactors for strontium capture in continuous flow. Microporous and Mesoporous Materials, 2016, 232: 39–52
CrossRef Google scholar
[28]
RobsonHLillerudK P. Verified Synthesis of Zeolitic Materials, 2nd. rev. ed. International Zeolite Association. Amsterdam, Netherlands, 2001
[29]
Awala H , Gilson J P , Retoux R , Boullay P , Goupil J M , Valtchev V , Mintova S . Template-free nanosized faujasite-type zeolites. Nature Materials, 2015, 14(4): 447–451
CrossRef Google scholar
[30]
Mintova S , Jaber M , Valtchev V . Nanosized microporous crystals: emerging applications. Chemical Society Reviews, 2015, 44(20): 7207–7233
CrossRef Google scholar
[31]
Zhang C , Wu Q , Lei C , Han S , Zhu Q , Maurer S , Dai D , Parvulescu A N , Müller U , Meng X . . An efficient, rapid, and non-centrifugation synthesis of nanosized zeolites by accelerating the nucleation rate. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2018, 6(42): 21156–21161
CrossRef Google scholar
[32]
Lagergren S K . About the theory of so-called adsorption of soluble substances. Sven. Vetenskapsakad. Handingarl, 1898, 24: 1–39
[33]
Ho Y S , McKay G . Pseudo-second order model for sorption processes. Process Biochemistry, 1999, 34(5): 451–465
CrossRef Google scholar
[34]
Weber W J Jr , Morris J C . Kinetics of adsorption on carbon from solution. Journal of the Sanitary Engineering Division, 1963, 89(2): 31–59
CrossRef Google scholar
[35]
Xue Z , Ma J , Hao W , Bai X , Kang Y , Liu J , Li R . Synthesis and characterization of ordered mesoporous zeolite LTA with high ion exchange ability. Journal of Materials Chemistry, 2012, 22(6): 2532–2538
CrossRef Google scholar
[36]
Datta S J , Moon W K , Choi D Y , Hwang I C , Yoon K B . A novel vanadosilicate with hexadeca-coordinated Cs+ ions as a highly effective Cs+ remover. Angewandte Chemie, 2014, 126(28): 7331–7336
CrossRef Google scholar
[37]
Yang H , Luo M , Luo L , Wang H , Hu D , Lin J , Wang X , Wang Y , Wang S , Bu X . . Highly selective and rapid uptake of radionuclide cesium based on robust zeolitic chalcogenide via stepwise ion-exchange strategy. Chemistry of Materials, 2016, 28(23): 8774–8780
CrossRef Google scholar
[38]
Thomas H C . Heterogeneous ion exchange in a flowing system. Journal of the American Chemical Society, 1944, 66(10): 1664–1666
CrossRef Google scholar
[39]
Loewenstein W . The distribution of aluminum in the tetrahedral of silicates and aluminates. American Mineralogist, 1954, 39(1–2): 92–96
[40]
Wang H , Holmberg B A , Yan Y . Synthesis of template-free zeolite nanocrystals by using in situ thermoreversible polymer hydrogels. Journal of the American Chemical Society, 2003, 125(33): 9928–9929
CrossRef Google scholar
[41]
Ishikawa Y , Tsukimoto S , Nakayama K S , Asao N . Ultrafine sodium titanate nanowires with extraordinary Sr ion-exchange properties. Nano Letters, 2015, 15(5): 2980–2984
CrossRef Google scholar
[42]
Liu C , Chen L , Ye Z , Li C , Yin X , Wang X , Wei Y . Pellet silica-based titanate adsorbents with high selectivity for strontium removal from synthetic radioactive solutions. Journal of Sol-Gel Science and Technology, 2019, 91(2): 273–285
CrossRef Google scholar
[43]
Zhang J , Chen L , Dai X , Zhu L , Xiao C , Xu L , Zhang Z , Alekseev E V , Wang Y , Zhang C . . Distinctive two-step intercalation of Sr2+ into a coordination polymer with record high 90Sr uptake capabilities. Chem, 2019, 5(4): 977–994
CrossRef Google scholar
[44]
Zhang M , Gu P , Yan S , Dong L , Zhang G . Na/Zn/Sn/S (NaZTS): quaternary metal sulfide nanosheets for efficient adsorption of radioactive strontium ions. Chemical Engineering Journal, 2020, 379: 122227
CrossRef Google scholar
[45]
Zhao X , Meng Q , Chen G , Wu Z , Sun G , Yu G , Sheng L , Weng H , Lin M . An acid-resistant magnetic Nb-substituted crystalline silicotitanate for selective separation of strontium and/or cesium ions from aqueous solution. Chemical Engineering Journal, 2018, 352: 133–142
CrossRef Google scholar

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

This research was financially supported by the institute of Civil Miltary Technology cooperation funded by the Defense Acquisition Program Administration and Ministry of Trade, Industry and Energy of Korea Government under grant No. 22-CM-BR-14.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-024-2449-6 and is accessible for authorized users.

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