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Issue 108, 2016
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Sorption behaviour of Pu4+ and PuO22+ on amido amine-functionalized carbon nanotubes: experimental and computational study

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Abstract

Amido amine-functionalized multi-walled carbon nanotubes (MWCNT-AA) were used for efficient and selective solid phase separation of plutonium(IV) and plutonium(VI). Langmuir, Freundlich, Dubinin–Radushkevich (D–R), and Tempkin isotherms were employed for understanding the sorption mechanism and Lagergren first order kinetics, an intra-particle diffusion model, and pseudo second order kinetics were applied to understand the sorption kinetics. The sorption proceeded through monolayer coverage of MWCNT-AA with capacities of 91.2 mg g−1 and 89.4 mg g−1 for Pu4+ and PuO22+, respectively following a Langmuir isotherm while the sorption kinetics followed a pseudo second order reaction with rate constants of 3.86 × 10−5 and 3.19 × 10−5 g mg−1 min−1 for Pu4+ and PuO22+ respectively. This MWCNT-AA showed high radiolytic stability and a method was developed for almost quantitative back extraction of plutonium in both the oxidation states from MWCNT-AA. Finally, the sorbent MWCNT-AA was employed for processing synthetic high level waste solution obtained from a research reactor origin. Moreover, density functional theory calculation was performed to examine the coordination and interaction behaviour of Pu4+ and PuO22+ ions towards MWCNT-AA. The present DFT study reveals that Pu is deca-coordinated (two from each of four nitrates and one AA) in the case of Pu4+ and octa-coordinated (two from each of two nitrates and one AA, and one from each of two oxo groups) in PuO22+. The calculated free energy of complexation was found to be almost three times higher for Pu4+ than PuO22+ both in the gas and aqueous phase, which thus confirms the experimentally observed higher sorption of Pu4+ compared to PuO22+ by MWCNT-AA.

Graphical abstract: Sorption behaviour of Pu4+ and PuO22+ on amido amine-functionalized carbon nanotubes: experimental and computational study

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Publication details

The article was received on 29 Sep 2016, accepted on 29 Oct 2016 and first published on 31 Oct 2016


Article type: Paper
DOI: 10.1039/C6RA24184K
Citation: RSC Adv., 2016,6, 107011-107020

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    Sorption behaviour of Pu4+ and PuO22+ on amido amine-functionalized carbon nanotubes: experimental and computational study

    P. Kumar, A. Sengupta, A. K. Singha Deb, K. Dasgupta and Sk. M. Ali, RSC Adv., 2016, 6, 107011
    DOI: 10.1039/C6RA24184K

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