Selective Separation of Zr(IV) from Simulated High-Level Liquid Wastes by Zeolites

Hu, Yifu; Hao, Wenfeng; Wang, Wentao; Zhang, Ye; Chen, Qi; Yan, Taihong

doi:10.1080/07366299.2023.2231493

Cited by 2 publications

(6 citation statements)

References 67 publications

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“…In theory, the adsorption capacity of Zr(IV) will also change with the difference in silicon hydroxyl group, so it is necessary to study the types of silicon hydroxyl groups on the surface of silica adsorbents. The utilization of solid-state 29 Si NMR to identify surface silicon hydroxyl groups within different silica gels was first reported by Maciel et al [49][50][51]. The 29 Si NMR spectrum revealed isolated silanols at approximately 100 ppm and geminal silanols at around 91 ppm.…”

Section: Mechanismmentioning

confidence: 95%

“…The binding energies were referenced from the carbon C1s line at 284.8 eV originating from adventitious carbon. 29 Si MAS NMR spectroscopy was conducted using a Bruker Ascend III 400 WB. The bath shaker (SHA-B) was procured from Hangzhou Qinlai Experimental Instrument Co., Ltd (Hangzhou, China).…”

Section: Characterizationmentioning

confidence: 99%

“…The 29 Si NMR spectrum revealed isolated silanols at approximately 100 ppm and geminal silanols at around 91 ppm. The resonance areas in each 29 Si NMR spectrum were obtained through a curve fitting routine, and then deconvolution was performed (Figure S2). The relative isolated silanol area (%I) is the resonance area of ~100 ppm (I) divided by the sum of I and the ~91 ppm geminal silanol resonance areas (G) (Table 5).…”

Section: Mechanismmentioning

confidence: 99%

“…Over the past few decades, researchers have developed diverse adsorbents [ 10 , 11 ], including organic ion exchange resins [ 12 , 13 , 14 , 15 , 16 ], sodium alginate gel [ 17 ], silicon-based materials [ 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 ], zeolites [ 29 ], and hydrous ferric oxide [ 30 ]. However, most of these adsorbents suffer from poor selectivity, poor acid resistance (only being effective in a narrow pH range in most cases), a low adsorption capacity, long adsorption equilibrium times, and poor radiation resistance, which limits their practical application.…”

Section: Introductionmentioning

confidence: 99%

“…The experimental data were subjected to fitting using both a kinetic model and a thermodynamic model to further elucidate the adsorption properties concerning Zr(IV). Finally, 29 Si magic-angle spinning nuclear magnetic resonance spectra ( 29 Si MAS NMR) and X-ray photoelectron spectroscopy (XPS) techniques were used to analyze the interaction mechanism between mesoporous silicas and Zr(IV) during the adsorption process.…”

Section: Introductionmentioning

confidence: 99%

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Selective Separation of Zr(IV) from Simulated High-Level Liquid Waste by Mesoporous Silica

Hu,

Bai,

Chen

et al. 2023

Nanomaterials

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The efficient separation of Zr(IV) ions from strong acidic and radioactive solutions is a significant challenge, especially in the context of the aqueous reprocessing of nuclear fuels. The complexity of such solutions, which are often characterized by high acidity and the presence of radioactive elements, poses formidable challenges for separation processes. Herein, several mesoporous silicas (HMS, MCM-41, KIT-6, and SiO2-70 Å) with excellent acid and radiation resistance properties were employed as sorbents to remove Zr(IV) ions from simulated high-level liquid waste. The batch experiments were designed to investigate the influence of adsorption time, HNO3 concentration, initial Zr(IV) concentration, adsorbent dosage, and temperature on the adsorption behavior of Zr(IV). The results indicate that the adsorption equilibrium time of mesoporous silica materials was approximately 8 h, and all the adsorption processes followed the pseudo-second-order kinetics equation. The isotherms of Zr(IV) adsorption by KIT-6 exhibited good agreement with the Langmuir model, while the Freundlich model could be utilized to fit the adsorption on HMS, MCM-41, and SiO2-70 Å. The adsorption capacity of MCM-41 for Zr(IV) in 3 mol/L HNO3 was 54.91 mg/g, which is three times the adsorption capacity reported for commercial silica gel (17.91 mg/g). The thermodynamic parameters indicate that the adsorption processes for zirconium are endothermic reactions. Furthermore, the mesoporous silicas exhibited a pronounced selectivity in the adsorption of Zr(IV) within a simulated high-level liquid waste containing 10 co-existing cations (3 mol/L HNO3). This suggests that mesoporous silicas have great potential for Zr(IV) removal in actual radioactive liquids with high acidity during spent fuel reprocessing.

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