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

doi:10.1007/s11705-024-2449-6

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (9) : 98 https://doi.org/10.1007/s11705-024-2449-6

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

Hyungmin Jeon¹, Susung Lee¹, Jeong-Chul Kim², Minkee Choi¹(

)

¹. Department of Chemical and Biomolecular Engineering (BK21 Four), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
². Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS), Daejeon 34141, Republic of Korea

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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.

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

Corresponding Author(s): Minkee Choi

Just Accepted Date: 19 April 2024 Issue Date: 18 July 2024

Cite this article:

Hyungmin Jeon,Susung Lee,Jeong-Chul Kim, et al. Nanocrystalline low-silica X zeolite as an efficient ion-exchanger enabling fast radioactive strontium capture[J]. Front. Chem. Sci. Eng., 2024, 18(9): 98.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2449-6
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I9/98

Tab.1 Physical and chemical properties of the zeolites

Fig.1 (a) XRD patterns and (b) N2 adsorption-desorption isotherms at 77 K for the zeolite samples. SEM images of (c) NaA, (d) LSX-1, (e) LSX-2, and (f) LSX-3.

Fig.2 (a) Kinetics of Sr²⁺-exchange for the zeolites in a solution with a Sr²⁺ concentration of 100 mg·L^–1. Pseudo-second order kinetic fitting results are indicated as trend lines. (b) Plots of the normalized Sr²⁺ uptake vs the square root of time.

Tab.2 Fitting results of the pseudo-second order model for Sr²⁺-exchange over the synthesized zeolites

Fig.3 Sr²⁺-exchange isotherms of the zeolites. Langmuir isotherm fitting results are represented as solid trend lines.

Tab.3 Langmuir fitting results for Sr²⁺-exchange isotherms

Fig.4 Distribution coefficient (K_d) and Sr²⁺ removal (%) of LSX-3 and NaA in aqueous solutions containing 1 mg·L^–1 Sr²⁺ and various molar ratios competing cations (a) Na⁺ and (b) Ca²⁺. (c) Capability of LSX-3 and NaA zeolites in removing 1 mg·L^–1 Sr²⁺ in deionised water, simulated groundwater, and simulated seawater.

Fig.5 Comparison of maximum Sr²⁺-exchange capacity and required equilibrium time for LSX-3, NaA, and various ion-exchangers in the literature.

Tab.4 Thomas model fitting results and the resulting parameters for the column experiments

Fig.6 Fixed-bed column adsorption of Sr²⁺ using NaA and LSX-3 zeolites (initial Sr²⁺ concentration: 10 mg·L^–1, flow rate: 60 BV·h^–1).

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