The Uranium from Seawater Program at the Pacific Northwest National Laboratory: Overview of Marine Testing, Adsorbent Characterization, Adsorbent Durability, Adsorbent Toxicity, and Deployment Studies

Gill, Gary A.; Kuo, Lih; Janke, Christopher J.; Park, Jiyeon; Jeters, Robert T.; Bonheyo, George T.; Pan, Horng Bin; Wai, Chien M.; Khangaonkar, Tarang; Bianucci, Laura; Wood, Jordana R.; Warner, Marvin G.; Peterson, Sonja; Abrecht, David G.; Mayes, Richard T.; Tsouris, Costas; Oyola, Yatsandra; Strivens, Jonathan E.; Schlafer, Nicholas J.; Addleman, Shane Raymond; Chouyyok, Wilaiwan; Das, Sadananda; Kim, Jungseung; Buesseler, Ken O.; Breier, Crystal; D’Alessandro, Evan K.

doi:10.1021/acs.iecr.5b03649

Cited by 123 publications

(115 citation statements)

References 55 publications

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“…Theu ranium adsorption capacity of SSUP fiber was reached more quickly than that of all of the previously available fiber adsorbents,which usually take days or weeks for saturation in high-concentration uranium spiked simulated seawater. [3,25] Thea dsorption mechanism analysis showed that the adsorption behavior of SSUP fiber fitted well with the pseudo-second-order kinetic model and that SSUP fiber adsorbed uranium mainly by chemical adsorption (Figure 3b;Figure S9). Based on the mechanism for uranium binding,e ach of the SUP protein only immobilized one molecule of uranyl ion.…”

Section: Angewandte Chemiementioning

confidence: 78%

Ultrafast and Highly Selective Uranium Extraction from Seawater by Hydrogel‐like Spidroin‐based Protein Fiber

et al. 2019

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Fort he practical extraction of uranium from seawater,a dsorbents with high adsorption capacity,f ast equilibrium rate,h igh selectivity,a nd long service life are needed. Herein, ac himeric spidroin-based super uranyl-binding protein (SSUP) fiber was designed by fusing the gene of super uranyl-binding protein (SUP) with the gene of spidroin. SUP endowed the SSUP fiber with high affinity and selectivity to uranium, and spidroin gave the SSUP fiber with high mechanical strength and high reusability.T he wet SSUP fiber is aw ater-rich hydrogel-like structure,w hich provided abundant hydrophilic intermolecular space for the entrance of uranyl ions,a nd could accelerate the rate for uranium adsorption. In seawater,t he SSUP fiber achieved ab reakthrough uranium extraction capacity of 12.33 mg g À1 with an ultrashort equilibration time of 3.5 days,suggesting that SSUP fiber might be ap romising adsorbent for uranium extraction from the natural seawater.Uranium is ak ey element of the nuclear-energy industry, which accounts for 13 %o ft he worldse lectricity supply without greenhouse gas generation. [1] Theocean, with atotal amount of 4.5 billion tons of uranium, is estimated to contain thousands of times of more uranium than terrestrial uranium reserves. [2] As ac onsequence of low solubility,t he concentration of soluble uranium in seawater is only 3.3 ppb (mgkg À1 ). [3] In addition, the coexisting marine interference metal ions,e specially vanadium, can seriously compete with uranium and make the extraction of uranium from seawater challenging. [4] Meanwhile,t he complex marine environment can severely hazard the adsorbents and reduces the service life of adsorbents.T hus,t he development of uranium adsorbents with high loading capacity,h igh specificity,f ast saturation time,h igh reusability,a nd strong mechanical property,are highly desirable.Amidoxime-based polymer adsorbents exhibit high potential because of their relatively high selectivity and binding capacity and have been used in uranium recovery from seawater since the 1980s. [2a] Fiber adsorbents based on the amidoxime group achieved the highest reported uranium extraction capacities of 1089 mg g À1 in uranium-spiked simulated seawater and 9.59 mg g À1 in real seawater. [5] The polymer fiber adsorbents are thus thought to be the optimal strategy for industrial recovery of uranium from seawater. [3, 6] However,t he saturation time of amidoxime-based polymer adsorbents is usually 4to8weeks in natural seawater, [7] which significantly reduces the efficiency and increases the economic cost for uranium extraction. Based on ah alf-wave rectified alternating current electrochemical (HW-ACE) method, the uranium extraction kinetics and capacity were enhanced to 1932 mg g À1 in 1000 ppm (mg kg À1 )u ranium spiked simulated seawater. [8] Recently,i norganic oxides/ sulfides, [9] metal-organic frameworks, [10] porous organic polymers, [11] covalent organic frameworks, [12] porous aromatic frameworks, [13] and carbon-based adsorbents [14] have been developed...

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Section: Angewandte Chemiementioning

confidence: 78%

Ultrafast and Highly Selective Uranium Extraction from Seawater by Hydrogel‐like Spidroin‐based Protein Fiber

et al. 2019

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“…Uranium and V adsorption experiments were conducted using a flow‐through column system using freshly filtered (0.45 μm) seawater from Sequim Bay, Washington . Seawater temperature was carefully controlled at 8, 20, and 31 °C.…”

Section: Resultsmentioning

confidence: 99%

“…Since the exposure experiments were conducted using a flow‐through system, the adsorbate concentrations ( C ) are the U and V concentrations in seawater. A 20‐month average of U and V concentrations in Sequim Bay seawater, normalized to a salinity of 35 psu, resulted in concentrations of 3.13 and 2.08 μg L −1 for U and V, respectively . Modelled saturation capacities from Table were used for Q .…”

Section: Resultsmentioning

confidence: 99%

“…Evidence to support the temperature effects observed in laboratory flow‐through column studies were obtained at a warm‐water field test site on Broad Key Island, Florida. AF1 adsorbent was exposed in a flow‐through channel (flume) system with filtered seawater from southern Biscayne Bay . The seawater temperature averaged 30.1 ± 0.7 °C.…”

Section: Resultsmentioning

confidence: 99%

“…Recently, significant improvements in adsorption capacity have been achieved for extraction of U from seawater using amidoxime‐based polymeric adsorbents ,,. Reported U adsorption loading in real seawater tests (20 °C, salinity 35 psu, 56 days of exposure) have reached 5.96 ± 0.29 g U (kg adsorbent) −1 , with a saturation capacity of 9.84 ± 0.48 g U (kg adsorbent) −1 . The uranium uptake rate of the adsorbent can be higher in ocean currents of higher velocity than that used in laboratory tests (i. e., 2 cm/s), yielding a better 56‐day adsorption performance .…”

Section: Introductionmentioning

confidence: 99%

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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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Rational Design of Porous Nanofiber Adsorbent by Blow‐Spinning with Ultrahigh Uranium Recovery Capacity from Seawater

Yuan

Zhao

Wen

et al. 2018

Adv Funct Materials

212

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Highly efficient recovery of uranium from seawater is of great concern because of the growing demand for nuclear energy. The use of amidoximebased polymeric fiber adsorbents is considered to be a promising approach because of their relatively high specificity and affinity to uranyl. The surface area, hydrophility, and surface charge of the adsorbent are reported to be critical factors that influence uranium recovery efficiency. Here, a porous amidoxime-based nanofiber adsorbent (SMON-PAO) that exhibits the highest uranium recovery capacity among the existing fiber adsorbents both in 8 ppm uranium spiked seawater (1089.36 ± 64.31 mg-U per g-Ads) and in natural seawater (9.59 ± 0.64 mg-U per g-Ads) is prepared by blow spinning. These nanofibers are obtained by compositing polyacrylamidoxime with montmorillonite and exhibit the increased surface area and more exposed functional amidoxime moieties for uranyl adsorption. The residual montmorillonite enhances the hydrophility and reduces the negative surface charge, thereby increasing the contact of the adsorbent with seawater and reducing the charge repulsion between negative amidoxime group and negative uranyl species ([UO 2 (CO 3 ) 3 ] 4− ). The finding of this study indicates that rational design of uranium recovery adsorbents by comprehensive utilizing the key factors that influence uranium recovery performance is a promising approach for developing economically feasible uranium recovery materials.

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The Uranium from Seawater Program at the Pacific Northwest National Laboratory: Overview of Marine Testing, Adsorbent Characterization, Adsorbent Durability, Adsorbent Toxicity, and Deployment Studies

Cited by 123 publications

References 55 publications

Ultrafast and Highly Selective Uranium Extraction from Seawater by Hydrogel‐like Spidroin‐based Protein Fiber

Ultrafast and Highly Selective Uranium Extraction from Seawater by Hydrogel‐like Spidroin‐based Protein Fiber

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

Rational Design of Porous Nanofiber Adsorbent by Blow‐Spinning with Ultrahigh Uranium Recovery Capacity from Seawater

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