Synthesis of polyamidoxime-functionalized nanoparticles for uranium(VI) removal from neutral aqueous solutions

Huang, Li; Zhang, Lixia; Hua, Daoben

doi:10.1007/s10967-015-3988-6

Cited by 22 publications

(12 citation statements)

References 52 publications

(69 reference statements)

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“…Introduction of competing cations (Na + , Mg 2+ , Zn 2+ , Co 2+ , Fe 3+ , Pb 3+ , and Ni 2+ ) reduced adsorption efficiency from 4− 30% at pH 6, and a modest decrease in performance was observed over five recycles. 157 Related work by the same group reported preparation of bifunctional poly(ionic liquid) microspheres by applying a similar process. 158 Block copolymers of poly(N-vinylimidazole)-block-poly(St) were prepared by RAFT.…”

Section: Chemical Reviewsmentioning

confidence: 99%

“…The poly(AN) block can then be converted to poly(AO) with hydroxylamine, and the resulting poly(AO) -block -poly(St) can then be further polymerized into microspheres via emulsion polymerization of the poly(St) block with additional St or DVB (Figure ). This approach affords fine-tunability of the AO chain length through controlling the poly(AN) and poly(St) blocks, while the AO concentration can be modulated through varying the concentration of the poly(AO)- block -poly(St) in the emulsion polymerization step.…”

Section: Synthetic Polymersmentioning

confidence: 99%

Section: Synthetic Polymersmentioning

confidence: 99%

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Materials for the Recovery of Uranium from Seawater

et al. 2017

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More than 1000× uranium exists in the oceans than exists in terrestrial ores. With nuclear power generation expected to increase over the coming decades, access to this unconventional reserve is a matter of energy security. With origins in the mid-1950s, materials have been developed for the selective recovery of seawater uranium for more than six decades, with a renewed interest in particular since 2010. This review comprehensively surveys materials developed from 2000-2016 for recovery of seawater uranium, in particular including recent developments in inorganic materials; polymer adsorbents and related research pertaining to amidoxime; and nanostructured materials such as metal-organic frameworks, porous-organic polymers, and mesoporous carbons. Challenges of performing reliable and reproducible uranium adsorption studies are also discussed, as well as the standardization of parameters necessary to ensure valid comparisons between different adsorbents.

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Section: Chemical Reviewsmentioning

confidence: 99%

Section: Synthetic Polymersmentioning

confidence: 99%

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Materials for the Recovery of Uranium from Seawater

et al. 2017

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“…There are multiple challenges which hinder deployment of the technology for seawater uranium extraction, driven by the low (∼3 ppb) concentration in seawater and the stability of the uranyl tris-carbonato complex UO 2 (CO 3 ) 3 4– . , Recent efforts within the scientific community have begun to address cardinal environmental effects on the performance of amidoxime-based adsorbents. These efforts include understanding of ion-competition for binding sites, − temperature dependence of uranium adsorption, − the effect of current velocity on passive adsorption, and the effects of pH on the uranyl ion–amidoxime interaction. − An unexplored factor, the effects of dissolved organic matter (DOM) with amidoxime-based adsorbents, is the next pragmatic area of consideration due to the ubiquitous presence of DOM in natural waters.…”

Section: Introductionmentioning

confidence: 99%

Assessment of Impacts of Dissolved Organic Matter and Dissolved Iron on the Performance of Amidoxime-Based Adsorbents for Seawater Uranium Extraction

Kuo

Pan

Strivens

et al. 2019

Ind. Eng. Chem. Res.

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One critical challenge of the development of seawater uranium extraction is to make uranium adsorbents perform well in the complex real seawater matrix, which is comprised of many competing ions and natural organic substances. Here, we conducted a systematic study using a continuous-flow seawater flume system to assess the potential impacts of dissolved organic matter (DOM) and dissolved iron on the uranium uptake performance, including adsorbent reusability, of amidoxime-based adsorbents. In the 28-day exposure, the adsorbent exposed in dissolved Fe-spiked seawater (low DOM/high Fe) and humic acid-spiked seawater (high DOM/high Fe) showed lower uranium adsorption loadings (73% and 56% of adsorption loading, respectively) than the same adsorbent exposed in seawater without spiking (low DOM/low Fe). The uranium adsorption loading of the reused adsorbent (after uranium stripping by a mild bicarbonate elution) in the dissolved Fe-spiked seawater dropped substantially to only 24% of the loading in the unspiked clean seawater counterpart, while not much change was observed in the performance of the adsorbent exposed to the humic acid-spiked seawater. Fourier transform infrared signatures of adsorbents suggest that the amidoxime ligands in the adsorbent exposed to dissolved Fe-spiked seawater had more severe degradation than the adsorbents exposed to humic acid-spiked seawater and unspiked clean seawater. Unlike the adsorbent exposed to dissolved Fe-spiked seawater, the adsorbent exposed to humic acidspiked seawater did not adsorb an elevated level of Fe compared to the adsorbent in the unspiked clean seawater. This suggests that the species of Fe in the humic acid-spiked seawater (primarily humic acid bound Fe) did not interact with the amidoximebased adsorbent, while the Fe species in the Fe-spiked seawater strongly interacted with the adsorbent and caused significant degradation of amidoxime ligands. On the other hand, highly variable uranium adsorption loadings were observed in the adsorbent in contact with humic acid-spiked seawater, but not in the adsorbents exposed to dissolved Fe-spiked seawater and seawater without spiking. Our observations indicate that seawater receiving high inputs of DOM and dissolved Fe, such as coastal waters, is not ideal for efficient extraction of uranium.

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“…A key feature in the development of this method is the selective sequestration of U(VI), and our initial polymer matrix was functionalized with amidoxime (AO) functional groups. , Amidoximated polyacrylonitrile (AO-PAN) mats were chosen because this surface chemistry has been previously used to sequester the uranyl ion (U VI O 2 2+ ) at very low concentrations from seawater, even in the presence of much higher concentrations of competing metal ions. − Advanced AO-based extractants have been recently explored for use in U(VI) extraction, such as nanoparticles, , ionic liquids, metal–organic frameworks, covalent organic frameworks, etc. From an engineering prospective, the nitrile groups on the PAN can readily be converted to amidoxime and the absorbents that can be fabricated on a large scale …”

Section: Introductionmentioning

confidence: 99%

Uranyl Speciation on the Surface of Amidoximated Polyacrylonitrile Mats

et al. 2020

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Naturally occurring uranium is a widespread contaminant present in the water resources around the abandoned uranium mines in the southwest United States. A novel method for rapid uranium detection has been recently developed that relies on the sequestering of uranium by amidoximated polyacrylonitrile (AO-PAN) polymer mats and uses the Raman-active (ν1) symmetric stretch as the signal. The Raman signals obtained from uranium bearing AO-PAN were challenging to interpret due to an unknown uranyl speciation on the surface of the mats. Herein, we provide the synthesis and structural characterization of six model coordination compounds that contain acetamidoxime/benzamidoxime (AAO/BAO) coordinated to the uranyl cation: [UO2(η1-AAO)(NO3)2(H2O)] (1), [UO2(η1-AAO)2(NO3)2] (2), [UO2(η2-BAO)2(CH3OH)2] (3), [(UO2)3(η2-BAO)3(μ2-NO3)3] (4), [(UO2)4(μ3-O)2(μ2-BAO)4(η1-BAO)4(H2O)2](NO3)4 (5), and [(UO2)4(μ3-O)2(μ2-BAO)4(η1-BAO)6Na(NO3)2](NO3)3 (6). Solid-state Raman spectra of 1–6 showed dramatic differences in the uranyl ν1 symmetric stretch depending on the coordination of the amidoxime functional group. The assignments made from the solid-state Raman spectra were used to deconvolute the solution-state Raman spectra of uranyl–acetamidoxime/benzamidoxime methanol solutions at different metal to ligand molar ratios. At low molar ratios (1 U:1 AAO/BAO and 1 U:2 AAO/BAO) the dominant species is the uranyl coordinated via the η1-oxygen atom of the oxime group, while at high molar ratios (1 U:3 AAO/BAO and 1 U:4 AAO/BAO) the dominant species are a tetrameric uranyl−μ3-O-η1-amidoxime complex similar to compounds 5 and 6 and a uranyl−η2-amidoxime complex similar to compounds 3 and 4. Solid-state Raman spectra showed good agreement with Raman signals obtained from the uranyl–AO-PAN mats, demonstrating that binding motifs between uranyl and amidoxime in compounds 5 and 6 are the most representative of the uranyl species on the surface of the AO-PAN mats.

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Synthesis of polyamidoxime-functionalized nanoparticles for uranium(VI) removal from neutral aqueous solutions

Cited by 22 publications

References 52 publications

Materials for the Recovery of Uranium from Seawater

Materials for the Recovery of Uranium from Seawater

Assessment of Impacts of Dissolved Organic Matter and Dissolved Iron on the Performance of Amidoxime-Based Adsorbents for Seawater Uranium Extraction

Uranyl Speciation on the Surface of Amidoximated Polyacrylonitrile Mats

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