Origin of the unusually strong and selective binding of vanadium by polyamidoximes in seawater

Ivanov, Alexander S.; Leggett, Christina J.; Parker, Bernard F.; Zhang, Zhicheng; Arnold, John; Dai, Sheng; Abney, Carter W.; Bryantsev, Vyacheslav S.; Rao, Linfeng

doi:10.1038/s41467-017-01443-1

Cited by 131 publications

(84 citation statements)

References 46 publications

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“…As illustrated in Figure 4f, the uptake of Ca and Mg are very fast in the first 2 weeks then slow down to a near plateau after 4 weeks. [50] Thus, the adsorption results once again indicate that cyclic imide dioxime are the predominant component of the blow spun PIDO NF adsorbents. The uptake of V reaches 14.35 ± 1.41 mg-V per g-Ads after 8 weeks of exposure, which is almost two times higher than that of U.…”

Section: Field Test In Natural Seawatermentioning

confidence: 69%

Significantly Enhanced Uranium Extraction from Seawater with Mass Produced Fully Amidoximated Nanofiber Adsorbent

Wang

Song

Wen

et al. 2018

Advanced Energy Materials

248

166

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electricity on a large scale with ultralow greenhouse gases emission. [2] Uranium is the most critical ingredient for the production of nuclear power. In order for nuclear power to be a sustainable energy generation in the future, economically viable sources of uranium beyond terrestrial ores must be developed. [3] The oceans hold ≈4.5 billion tons of uranium, [4] making them a potential huge resource to support nuclear power production for hundreds of years. [5] All that is required is the ability to capture this element from seawater in cost-and energy-efficient ways. In the last decades, researchers worldwide have tried various methods to recover uranium from seawater and aqueous solution, such as coprecipitation, [6] ion-exchange, [7] adsorption via porous organic polymers, [8,9] and organic-inorganic hybrid adsorbents. [10][11][12][13][14][15][16] Among these technologies, the adsorption approach, particularly by using fiber-based adsorbents, is recognized as the most feasible process in terms of practicality, processability, cost, and environmental concerns. [3,17] In the 1990s, Japan Atomic Energy Agency (JAEA) research teams had successfully captured over 1083 g of uranium directly from ocean by using nonwoven fabric adsorbent, firmly establishing the practicality of uranium recovery from the oceans in appreciable quantities. [3,18] Uranium extraction from seawater via fiber adsorption has recentlyThe oceans contain hundreds of times more uranium than terrestrial ores. Fiber-based adsorption is considered to be the most promising method to realize the industrialization of uranium extraction from seawater. In this work, a pre-amidoximation with a blow spinning strategy is developed for mass production of poly(imide dioxime) nanofiber (PIDO NF) adsorbents with many chelating sites, excellent hydrophilicity, 3D porous architecture, and good mechanical properties. The structural evidences from 13 C NMR spectra confirm that the main functional group responsible for the uranyl binding is not "amidoxime" but cyclic "imidedioxime." The uranium adsorption capacity of the PIDO NF adsorbent reaches 951 mg-U per g-Ads in uranium (8 ppm) spiked natural seawater. An average adsorption capacity of 8.7 mg-U per g-Ads is obtained after 56 d of exposure in natural seawater via a flowthrough column system. Moreover, up to 98.5% of the adsorbed uranium can be rapidly eluted out and the adsorbent can be regenerated and reused for over eight cycles of adsorption-desorption. This new blow spun PIDO nanofabric shows great potential as a new generation adsorbent for uranium extraction from seawater.

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Section: Field Test In Natural Seawatermentioning

confidence: 69%

Significantly Enhanced Uranium Extraction from Seawater with Mass Produced Fully Amidoximated Nanofiber Adsorbent

Wang

Song

Wen

et al. 2018

Advanced Energy Materials

248

166

View full text Add to dashboard Cite

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“…Although the adsorption of other trace metal elements is much lower than that of uranium, vanadium adsorption is slightly higher than uranium adsorption (Table S3 and Figure S14, Supporting Information). This high vanadium uptake indicates that a portion of the amidoxime groups in the hydrogel transformed into cyclic imide‐dioxime groups, because, based on the reported literature, the amidoxime groups had only a fairly weak vanadium adsorption capacity. In contrast, the cyclic imide‐dioxime groups had much higher vanadium coordination than other metal elements (including uranium).…”

Section: Methodsmentioning

confidence: 85%

An Ion‐Crosslinked Supramolecular Hydrogel for Ultrahigh and Fast Uranium Recovery from Seawater

et al. 2020

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Large‐scale uranium extraction from seawater is a crucial but challenging part of nuclear power generation. In this study, a new ion‐crosslinked supramolecular Zn2+–poly(amidoxime) (PAO) hydrogel that can super‐efficiently adsorb uranium from seawater is explored. By simply mixing two solutions of zinc chloride and PAO, a supramolecular Zn2+–PAO hydrogel is achieved via the interaction between zinc cations and amidoxime anions. In contrast with existing amidoxime‐functionalized hydrogel‐based adsorbents having low PAO contents and fiber‐based adsorbents with weak hydrophilicity, the PAOs can be directly crosslinked using a small quantity of superhydrophilic zinc ion. Thus, a supramolecular hydrogel is formed, having both a high content of well‐dispersed PAOs and good hydrophilicity. Relative to reported adsorbents, this low‐cost hydrogel membrane exhibits outstanding uranium adsorption performance, reaching 1188 mg g-1 of MU/Mdry gel in 32 ppm uranium‐spiked water. More importantly, after immersion in natural seawater for only 4 weeks, the uranium extraction capacity of the Zn2+–PAO hydrogel membrane reaches 9.23 mg g-1 of MU/Mdry gel. This work can provide a general strategy for designing a new type of supramolecular hydrogel, crosslinked by various bivalent/multivalent cation‐crosslinkers and even many other superhydrophilic supramolecular crosslinkers, for the high‐efficient and massive extraction of uranium from seawater.

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“…Although the observed difference in enthalpies for V(V) binding between the two adsorbent formulations is statistically significant, the magnitudes are much smaller than those for U(VI) and the binding of V(V) to either adsorbent is essentially thermoneutral. Moreover, a recent analysis of seawater exposed AF1 and AI8 adsorbents using EXAFS found no difference in the coordination chemistry of V(V)‐amidoxime interaction in AF1 and AI8 adsorbents …”

Section: Resultsmentioning

confidence: 95%

Temperature Dependence of Uranium and Vanadium Adsorption on Amidoxime‐Based Adsorbents in Natural Seawater

et al. 2018

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Recent advances in the development of amidoxime‐based adsorbents have made it highly promising for seawater uranium extraction. However, there is a great need to understand the influence of temperature on the uranium sequestration performance of the adsorbents in natural seawater. Here the apparent enthalpy and entropy of the sorption of uranium (VI) and vanadium (V) with amidoxime‐based adsorbents were determined in natural seawater tests at 8, 20, and 31 °C that cover a broad range of ambient seawater temperature. The sorption of U was highly endothermic, producing apparent enthalpies of 57 ± 6.0 and 59 ± 11 kJ mol−1 and apparent entropies of 314 ± 21 and 320 ± 36 J K−1 mol−1, respectively, for two adsorbent formulations. In contrast, the sorption of V showed a much smaller temperature sensitivity, producing apparent enthalpies of 6.1 ± 5.9 and −11 ± 5.7 kJ mol−1 and apparent entropies of 164 ± 20 and 103 ± 19 J K−1 mol−1, respectively. This new thermodynamic information suggests that amidoxime‐based adsorbents will deliver significantly increased U adsorption capacities and improved selectivity in warmer waters. A separate field study of seawater uranium adsorption conducted in a warm seawater site (Miami, FL, USA) confirm the observed strong temperature effect on seawater uranium mining. This strong temperature dependence demonstrates that the warmer the seawater where the amidoxime‐based adsorbents are deployed the greater the yield for seawater uranium extraction.

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Origin of the unusually strong and selective binding of vanadium by polyamidoximes in seawater

Cited by 131 publications

References 46 publications

Significantly Enhanced Uranium Extraction from Seawater with Mass Produced Fully Amidoximated Nanofiber Adsorbent

Significantly Enhanced Uranium Extraction from Seawater with Mass Produced Fully Amidoximated Nanofiber Adsorbent

An Ion‐Crosslinked Supramolecular Hydrogel for Ultrahigh and Fast Uranium Recovery from Seawater

Temperature Dependence of Uranium and Vanadium Adsorption on Amidoxime‐Based Adsorbents in Natural Seawater

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