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Adsorption and desorption behavior of tetravalent zirconium onto a silica-based macroporous TODGA adsorbent in HNO3 solution
Authors:Yuanlai Xu  Seong-Yun Kim  Shigekazu Usuda  Yuezhou Wei  Keizo Ishii
Institution:1. Cyclotron and Radioisotope Center, Tohoku University, Aoba 6-3, Aramaki, Aoba-ku, Sendai, 980-8578, Japan
2. Department of Quantum Science and Energy Engineering, Graduate School of Engineering, Tohoku University, Aoba 6-6-1, Aramaki, Aoba-ku, Sendai, 980-8579, Japan
3. School of Nuclear Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China
Abstract:To understand the separation behavior of Zr(IV) in the partitioning process for high level liquid waste, a silica-based macroporous adsorbent (TODGA/SiO2-P) was prepared by impregnating N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide (TODGA) into a macroporous silica/polymer composite particles support (SiO2-P). Adsorption and desorption behavior of Zr(IV) from nitric acid solution onto silica-based TODGA/SiO2-P adsorbent were investigated by batch experiment. It was found that TODGA/SiO2-P showed strong adsorption affinity to Zr(IV) and this adsorption process reached equilibrium state around 6 h at 298 K. Meanwhile, HNO3 concentration had no significant effect on the adsorption of Zr(IV) above 1 M. From calculated thermodynamic parameters, this adsorption process could occur spontaneously at the given temperature and was confirmed to be an exothermic reaction. This adsorption process could be expressed by Langmuir monomolecular layer adsorption mode and the maximum adsorption capacity were determined to be 0.283 and 0.512 mmol/g for Zr(IV) at 298 and 323 K, respectively. In addition, more than 90 % of Zr(IV) adsorbed onto adsorbent could be desorbed with 0.01 M diethylenetriamine pentaacetic acid solution within 24 h at 298 K.
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