Design and synthesis of a novel bifunctional polymer with malonamide and carboxyl group for highly selective separation of uranium (VI)

Li, Yang; Li, Xu-Xin; Wang, Zeyang; Zhang, Fang; Wu, Qiang; Sha, Lei-Tao; Wang, Yun; Yan, Ze‐Yi

doi:10.1016/j.seppur.2022.122115

Cited by 34 publications

(7 citation statements)

References 49 publications

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“…The quasi-first-order kinetic model and the quasi-second-order kinetic model were adopted to explore the experimental data of the CA-PCDP@MNP adsorbed U(VI) with time; the fitting curve is exhibited in Figure 6b,c, and the fitting parameters are displayed in Table 1. It was observed that the fitting results of the quasi-second-order kinetic model (R 2 = 0.999) were better than that of the quasi-first-order kinetic model (R 2 = 0.718), and the equilibrium amount (qe, cal) calculated by the quasi-second-order kinetic model was also closer to the actual experimental equilibrium adsorption amount (qe, exp), suggesting that the CA-PCDP@MNP adsorption process followed a quasi-second-order kinetic model and that it was chemisorption [38]. This was because the CA-PCDP@MNPs had abundant oxygen-containing groups, which provided most of the adsorption actives [15,39].…”

Section: Adsorption Kineticsmentioning

confidence: 79%

Magnetic β-Cyclodextrin Polymer Nanoparticles for Efficient Adsorption of U(VI) from Wastewater

Zhong,

Lv,

Zhang

et al. 2023

Crystals

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It is a central issue to eliminate radioactive uranium (U(VI)) efficiently from water. In this manuscript, β-cyclodextrin was cross-linked with 2,3,5,6-tetrafluoro-1,4-benzenedicarbonitrile, and then a carboxylation reaction was used to prepare porous cross-linked polymers rich in carboxyl groups (CA-PCDPs). Subsequently, magnetic nanoparticles (MNPs) were loaded onto the CA-PCDPs via coprecipitation, and magnetic porous β-cyclodextrin polymer nanoparticles (CA-PCDP@MNPs) were successfully obtained, which were used for efficient elimination of U(VI) from nuclear wastewater solution. Moreover, SEM, FTIR, VSM, BET, and XRD were employed to investigate the CA-PCDP@MNP and found that it had a well-developed porous structure, high specific surface area, and abundant oxygen-containing functional groups (carboxyl, hydroxyl, C-O-C, Fe-O, etc.), providing sufficient active sites for chelating uranyl ions. Experiments illustrated that the CA-PCDP@MNP had efficient removal ability for U(VI), and the maximum theoretical adsorption amount for U(VI) reached 245.66 mg/g at pH 6.0 and 303 K. Moreover, the adsorption process was more suitable for the quasi second-order kinetic model and Langmuir adsorption isotherm model, indicating that the adsorption process was chemical adsorption. Meanwhile, the CA-PCDP@MNPs also exhibited fast response magnetic recovery ability and excellent regeneration and recycling ability. In addition, the data of the adsorption mechanism demonstrated that oxygen-containing functional groups, which were rich on the surface of CA-PCDP@MNPs, were the main binding active sites of U(VI). From the above results, it can be deduced that the CA-PCDP@MNP has a good application prospect in the practical application of nuclear wastewater treatment.

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Section: Adsorption Kineticsmentioning

confidence: 79%

Magnetic β-Cyclodextrin Polymer Nanoparticles for Efficient Adsorption of U(VI) from Wastewater

Zhong,

Lv,

Zhang

et al. 2023

Crystals

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“…The results showed that MCFCP always maintains high adsorption capacity and selectivity for uranyl ions in the presence of coexisting ions (Na(I), K(I), Rb(I), Cs(I), Mg(II), Ca(II), Sr(II), Ba(II), Zn(II), and Fe(III)) (Figure A). In the XPS spectrum, the new peaks of U 4f 5/2 (392.9 eV) and U 4f 7/2 (381.9 eV) suggested that UO 2 2+ was adsorbed on MCFCP (Figure B) . MIPAF (molecularly imprinted porous aromatic frameworks) -11c synthesized by Yuan et al had the highest selectivity in a mixture of 20 ppm UO 2 2+ and 2 ppm of each interfering ion (Na(I), Li(I), K(I), Ca(II), Mn(II), Mg(II), Co(II), Ni(II), Cu(II), Zn(II), Cd(II), Al(III), Fe(III), and Cr(VI)) in deionized water (Figure C).…”

Section: Uranium Enrichment and Separationmentioning

confidence: 99%

“…In the XPS spectrum, the new peaks of U 4f 5/2 (392.9 eV) and U 4f 7/2 (381.9 eV) suggested that UO 2 2+ was adsorbed on MCFCP (Figure 2B). 45 MIPAF (molecularly imprinted porous aromatic frameworks) -11c synthesized by Yuan et al had the highest selectivity in a mixture of 20 ppm UO 2 2+ and 2 ppm of each interfering ion (Na(I), Li(I), K(I), Ca(II), Mn(II), Mg(II), Co(II), Ni(II), Cu(II), Zn(II), Cd(II), Al(III), Fe(III), and Cr(VI)) in deionized water (Figure 2C). The U(VI) adsorption (Figure 2D) only slightly decreased from 14.5 mg/g to 14.2 mg/g after 10 cycles, indicating good recyclability.…”

Section: Pristine Organic Polymersmentioning

confidence: 99%

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Enrichment and Separation of Radionuclides by Organic Polymer Materials: A Review

Zhang,

Yang,

Rong

et al. 2024

ACS EST Eng.

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Nuclear power provides a chance for the decarbonization of global energyrelated emissions. However, the spent fuel produced by nuclear reactors contains various radionuclides, which require further disposal and treatment. Therefore, the enrichment and separation of radionuclides are of great significance for the recycling and utilization of resources. Organic polymer materials have attracted great attention due to their excellent physicochemical properties of rapid kinetics, high adsorption capacity, high selectivity, and diverse functionalization. This review provides an overview of the use of pristine polymers, functionalized polymers, and polymer-based composites for the highly efficient enrichment and separation of different kinds of radionuclides (i.e., U, Tc, I). The synthesis strategy, radionuclides enrichment and separation ability, and related mechanism are comprehensively summarized. The structure−property relationships in polymer-based materials that underpin their outstanding environmental remediation performance are also illustrated. Finally, the challenges and perspectives of polymer-based materials for future radionuclide separation and legacy nuclear waste management are reasonably proposed, aiming to design functional polymers for task-specific applications.

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“…The increasing demand of carbon-neutral and low-cost energy has caused nuclear energy to become an essential element in the overall composition of the current global power supply. − Accompanied by the high-speed development of nuclear energy, the environmental problems associated with used nuclear fuel have aroused great attention. − Of the spent fuel produced by modern light water reactors, over 98.5% of the components are mainly composed of U, Pu, and lanthanides (Ln) . However, it still contains less than 1 wt % of minor actinides (MA) including Am, Np, and Cm, which are responsible for long-standing radiotoxicity. − In order to improve the long-term management safety of nuclear waste, the partitioning-transmutation strategy (P&T) was emerged and recognized as a viable global option. , The proposed P&T initially partitioned the transuranic elements and long-lived fission products by the PUREX process using solvent extraction, , and they were subsequently subjected to neutron bombardment for transmutation into short-lived nuclides .…”

Section: Introductionmentioning

confidence: 99%

Selective Separation of Americium(III), Curium(III), and Lanthanide(III) by Aqueous and Organic Competitive Extraction

Wu,

Hao,

Liu

et al. 2023

Inorg. Chem.

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Adding hydrophilic ligands into aqueous solutions for the selective binding of actinides(III) is acknowledged as an advanced strategy in Ln(III)/ An(III) separation. In view of the recycling and radioactive waste disposal of the minor actinide, there remains an urgent need to design and develop the appropriate ligand for selective separation of An(III) from Ln(III). Herein, four novel hydrophilic ligands with hard−soft hybrid donors, derived from the pyridine and phenanthroline skeletons, were designed and synthesized as masking agents for selective complexation of An(III) in the aqueous phase. The known N,N,N′,N′-tetraoctyl diglycolamide (TODGA) was used as lipophilic extractant in the organic phase for extraction of Ln(III), and a new strategy for the competitive extraction of An(III) and Ln(III) was developed based on TODGA and the above hydrophilic ligands. The optimal hydrophilic ligand of N,N′-bis(2hydroxyethyl)-2,9-dicarboxamide-1,10-phenanthroline (2OH-DAPhen) displayed exceptional selectivity toward Am(III) over Ln(III), with the concentrations of HNO 3 ranging from 0.05 to 3.0 M. The maximum separation factors were up to 1365 for Eu/Am, 417.66 for Eu/Cm, and 42.38 for La/Am. The coordination mode and bonding property of 2OH-DAPhen with Ln(III) were investigated by 1 H NMR titration, UV−vis spectrophotometric titration, luminescence titration, FT-IR, ESI-HRMS analysis, and DFT calculations. The results revealed that the predominant species formed in the aqueous phase was a 1:1 ligand/metal complex. DFT calculations also confirmed that the affinity of 2OH-DAPhen for Am(III) was better than that for Eu(III). The present work using a competitive extraction strategy developed a feasible alternative method for the selective separation of trivalent actinides from lanthanides.

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Design and synthesis of a novel bifunctional polymer with malonamide and carboxyl group for highly selective separation of uranium (VI)

Cited by 34 publications

References 49 publications

Magnetic β-Cyclodextrin Polymer Nanoparticles for Efficient Adsorption of U(VI) from Wastewater

Magnetic β-Cyclodextrin Polymer Nanoparticles for Efficient Adsorption of U(VI) from Wastewater

Enrichment and Separation of Radionuclides by Organic Polymer Materials: A Review

Selective Separation of Americium(III), Curium(III), and Lanthanide(III) by Aqueous and Organic Competitive Extraction

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