Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture
Hyungmin Jeon, Susung Lee, Jeong-Chul Kim, Minkee Choi
Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture
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.
Sr2+ removal / low-silica X zeolite / nanocrystal / hydrogel / methyl cellulose
[1] |
Zhang Z , Cheng M , Xiao X , Bi K , Song T , Hu K Q , Dai Y , Zhou L , Liu C , Ji X .
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 .
CrossRef
Google scholar
|
[17] |
Zhang J , Chen L , Dai X , Chen L , Zhai F , Yu W , Guo S , Yang L , Chen L , Zhang Y .
CrossRef
Google scholar
|
[18] |
Tang X , Wang S , Zhang Z , Li Z , Wang L , Yuan L , Wang B , Sun J , Zheng L , Wang H .
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 .
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 .
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 .
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
|
/
〈 | 〉 |