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DOE OSTI2017

Recovery of Uranium from Seawater: Modified Polyacrylonitrile Fibers as Selective Extractants

A new bifunctional fiber has been prepared and found to have a significant loading capacity of uranium from real seawater. The fiber support is polyacrylonitrile and bifunctionality is provided by amidoxime and either diethylenetriamine (DETA) or ethylenediamine (EDA) ligands. The key feature is adjusting the hydrophilic /lipophilic balance within the fiber and this was best accomplished by partially acetylating or carboxylating EDA ligands. The bifunctional carboxylated EDA /AO fiber had a loading capacity of 3.83 mg U/g fiber at the Pacific Northwest National Laboratory with a 21 day contact time in real seawater.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2017

Development of Novel Porous Sorbents for Extraction of Uranium from Seawater

Climate disruption is one of the greatest crises the global community faces in the 21st century. Alarming increases in CO 2 , NO, SO 2 and particulate matter levels will have catastrophic consequences on the environment, food supplies, and human health if no action is taken to lessen their worldwide prevalence. Nuclear energy remains the only mature technology capable of continuous base-load power generation with ultralow carbon dioxide, nitric oxide, and sulfur dioxide emissions. Over the lifetime of the technology, nuclear energy outputs less than 1.5% the carbon dioxide emissions per gigawatt hour relative to coal—about as much as onshore wind power.1 However, in order for nuclear energy to be considered a viable option in the future, a stable supply of uranium must be secured. Current estimates suggest there is less than 100 years’ worth of uranium left in terrestrial ores (6.3 million tons) if current consumption levels remain unchanged.2 It is likely, however, that demand for nuclear fuel will rise as a direct consequence of the ratification of global climate accords. The oceans, containing approximately 4.5 billion tons of uranium (U) at a uniform concentration of ~3 ppb, represent a virtually limitless supply of this resource.3 Development of technologies to recover uranium from seawater would greatly improve the U resource availability, providing a U price ceiling for the current generation and sustaining the nuclear fuel supply for future generations. Several methods have been previously evaluated for uranium sequestration including solvent extraction, ion exchange, flotation, biomass collection, and adsorption; however, none have been found to be suitable for reasons including cost effectiveness, long term stability, and selectivity.4,5 While polymer beads and fibers have been functionalized with amidoxime functional groups to afford U adsorption capacities as high as 1.5 g U/kg,6 further discoveries are needed to make uranium extraction from seawater economically feasible.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Geologic Seawater Air Conditioning (GeoSWAC) System: Resource Assessment and Techno-Economic Evaluation in Puerto Rico

Puerto Rico's hot, humid climate drives a high and persistent demand for cooling, straining an aging and fuel-dependent energy grid while increasing peak electricity loads. Much of this challenge stems from inefficient air-conditioning systems operating in buildings without passive cooling design, making cooling both costly and vulnerable to disruption - especially during hurricanes. To address these issues, researchers evaluated a new alternative called Geologic Seawater Air Conditioning (GeoSWAC), which uses inland wells connected to naturally cold, deep seawater. By avoiding long offshore pipelines and energy-intensive refrigeration cycles, GeoSWAC can cut electricity use by 75-90%, reduce environmental impacts, and operate more reliably during power outages. A case study at the University of Puerto Rico's Rio Piedras campus found that GeoSWAC could deliver significantly lower levelized costs of cooling, reduced operational expenses, and improved water conservation compared to the campus's existing chilled-water plant. The system offers key advantages - including access to a constant cold heat sink, low pumping requirements, and enhanced resilience - for coastal regions such as Puerto Rico, the broader Caribbean, and Florida. However, its effectiveness depends heavily on site-specific geological conditions, such as subsurface connectivity and aquifer characteristics, which require detailed investigation. Future research should refine hydrogeological models, conduct performance and economic analyses, and address regulatory and permitting frameworks to support broader adoption of this promising technology.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2013

Adsorbent materials development and testing for the extraction of uranium from seawater

The extraction of uranium from seawater has been the focus of a research project for the U.S. Department of Energy to develop amidoxime functional group adsorbents using radiation-induced graphing on polymer-based fiber materials and subsequent chemical conversion of the radical sites to form the desired adsorbent material. Materials with promising uranium adsorption capacities were prepared through a series of parametric studies on radiation dose, time, temperature, graphing solutions, and properties of the base polymer materials. A laboratory screening protocol was developed to determine the uranium adsorption capacity to identify the most promising candidate materials for seawater testing. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2013

Energy balance for uranium recovery from seawater

The energy return on investment (EROI) of an energy resource is the ratio of the energy it ultimately produces to the energy used to recover it. EROI is a key viability measure for a new recovery technology, particularly in its early stages of development when financial cost assessment would be premature or highly uncertain. This paper estimates the EROI of uranium recovery from seawater via a braid adsorbent technology. In this paper, the energy cost of obtaining uranium from seawater is assessed by breaking the production chain into three processes: adsorbent production, adsorbent deployment and mooring, and uranium elution and purification. Both direct and embodied energy inputs are considered. Direct energy is the energy used by the processes themselves, while embodied energy is used to fabricate their material, equipment or chemical inputs. If the uranium is used in a once-through fuel cycle, the braid adsorbent technology EROI ranges from 12 to 27, depending on still-uncertain performance and system design parameters. It is highly sensitive to the adsorbent capacity in grams of U captured per kg of adsorbent as well as to potential economies in chemical use. This compares to an EROI of ca. 300 for contemporary terrestrial mining. It is important to note that these figures only consider the mineral extraction step in the fuel cycle. At a reference performance level of 2.76 g U recovered per kg adsorbent immersed, the largest energy consumers are the chemicals used in adsorbent production (63%), anchor chain mooring system fabrication and operations (17%), and unit processes in the adsorbent production step (12%). (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

A Beehive Inspired Hydrogen Photocatalytic Device Integrating a Carbo–Benzene Triptych Material for Efficient Solar Photo–Reduction of Seawater

The dream to produce green, clean and sustainable hydrogen from earth-abundant and free resources such as seawater and sunlight is highly motivating because of the interest for desirable economical and societal applications in energy. However, it remains challenging to develop an efficient and unassisted photocatalytic device to split seawater molecules with just sunlight without any external bias. For the first time, a such novel hierarchical material has been developed, based on thin film technology that integrates TiO 2 semiconductor layers, embedded gold nanoparticles and a photosensitive carbo-benzene layer. The design of the triptych device placing the photocatalyst in be-to-be increases the photoactive surface area by a factor 2. Its stability (>120 successive hours of hydrogen production and >5 days in a day/night representative alternation) and efficiency (STH 0.06%) are measured in NaCl-salted water. Here, the chloride ions act as hole scavengers and induce an increase of pH increasing in turn the sun-driven hydrogen production rate.

42 ENGINEERING↗

DOE OSTI2020

Differential effects of press vs. pulse seawater intrusion on microbial communities of a tidal freshwater marsh

Abstract Tidal freshwater marshes (TFMs) are threatened by seawater intrusion, which can affect microbial communities and alter biogeochemical processes. Here, we report on a long‐term, large‐scale manipulative field experiment that investigated continuous (press) and episodic (pulse, 2 months/yr) inputs of brackish water on microbial communities in a TFM. After 2.5 yr, microbial diversity was lower in press treatments than in control (untreated) plots whereas diversity in pulse plots was unaffected by brackish water additions. Sulfate reducer abundance increased in response to both press and pulse treatments whereas methanogens did not differ among treatments. Our results, along with other lab and field measurements that show reduced soil respiration and extracellular enzyme activity suggest that continuous seawater intrusion will decrease macrophyte C inputs that reduce bacterial diversity in ways that also diminish ecosystem carbon cycling.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2018

Techno-Economic Analysis of Magnesium Extraction from Seawater via a Catalyzed Organo-Metathetical Process

Magnesium (Mg) has many useful applications especially in various Mg alloys which can decrease weight while increasing strength. To increase the affordability and minimize environment consequence, a novel catalyzed organo-metathetical (COMET) process was proposed to extract Mg from seawater aiming to achieve significant reduction in total energy and production cost comparing with the melting salt electrolysis method currently adopted by US Mg LLC. A process flowsheet for a reference COMET process was set-up using Aspen Plus which included five key steps, anhydrous MgCl2 production, transmetallation, dibutyl Mg decomposition, n-BuLi regeneration, and LiCL electrolysis. The energy and production cost and CO2 emission were estimated based on the Aspen modeling using Aspen economic analyzer. Our results showed that it is possible to produce Mg from seawater with a production cost of $2.0/kg-Mg while consuming about 35.3 kWh/kg-Mg and releasing 7.0 kg CO2/kg-Mg. A simplified US Mg manufacturing process was also generated using Aspen and the cost and emission results were estimated for comparison purpose. Under our simulation conditions, the reference COMET process maintain a comparable CO2 emission rate and can save about 40% in production cost and save about 15% energy compared to the simplified US Mg process.

Liu, Jian (ORCID:0000000153297408)↗

DOE OSTI2023

Effect of chromium on corrosion resistance of Ni-Cr-Mo-Gd alloys in seawater

Neutron absorbing materials are being considered within commercial spent nuclear fuel disposal canisters to maintain nuclear subcriticality in storage. To select candidate alloys for the canisters, both neutron absorption and corrosion resistance should be considered. This work examines corrosion resistance of Ni-Cr-Mo-Gd alloys developed specifically for neutron absorption. The addition of Gd results in a secondary gadolinide phase (Ni 5 Gd) that significantly changes the corrosion properties. Testing was performed primarily in seawater at 30°C. Seawater was selected as the most prevalent terrestrial brine and is characterized by a high chloride concentration. Various electrochemical corrosion techniques were carried out to evaluate Ni-Cr-Mo-Gd alloys with different Cr compositions and investigate the role of Ni 5 Gd phase on corrosion behavior. C22 was included as a benchmark material, due to the similarity in composition and the significant corrosion data available. Here, test results showed a tendency to passivate over time which is attributed to dissolution of surface exposed Ni 5 Gd phase. Cross-sectional analysis indicated that dissolution could penetrate hundreds of micrometers deep under aggressive conditions. It was found that higher Cr variant (21.01%) showed much shallower impact, suggesting Cr prevented primary phase corrosion and thus reduced Ni 5 Gd phase dissolution. Acid pickling of the specimens showed much less dissolution for a higher Cr material and suggested some primary phase dissolution for the low Cr specimen. Acid pickled specimens showed positive shifts in the repassivation potential, suggesting increased surface passivation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2017

Materials for the Recovery of Uranium from Seawater

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-1950’s, 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. In conclusion, 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.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2015

Stripping Uranium from Seawater-Loaded Sorbents with the Ionic Liquid Hydroxylammonium Acetate in Acetic Acid for Efficient Reuse

A new stripping and recovery process was developed to harvest the uranium recovered from seawater with amidoxime-functionalized polyethylene fiber sorbents and allow reuse of the sorbent without loss of capacity and without the need to recondition the sorbent before reuse. Hydroxylammonium acetate ([NH 3 OH][OAc])/aqueous acetic acid (AcOH) solutions were used as weakly acidic stripping agents and the stripped uranium as a soluble acetate was further immobilized on shrimp shells. These solutions also stripped the vanadium and other metal ions coadsorbed, which reduce capacity through competition with uranium for sorbent binding and can resist stripping even by strong acids. [NH 3 OH][OAc]/AcOH was found to allow recovery of more than 85% of the uranium although at a substantial longer time than the current 0.5 M HCl-stripping solutions, (less than 12 h vs 48-72 h, respectively); however, the use of HCl severely compromises the capacity of the sorbent in subsequent reuse (a 50% lost was observed on the third reuse of the fiber). Both [NH 3 OH][OAc] and the acetic acid were necessary to achieve high uranium recovery without sacrificing the sorbent’s capacity on reuse. Finally, the ability to reuse the sorbent without pretreatment and with minimal capacity loss could be an important step toward making the extraction of uranium from seawater energy-efficient and economically viable.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2016

Highly Preorganized Ligand 1,10-Phenanthroline-2,9-dicarboxylic Acid for the Selective Recovery of Uranium from Seawater in the Presence of Competing Vanadium Species

Studies of the complexation of new promising ligands with uranyl (UO 2 2+ ) and other seawater cations can aid the development of more efficient, selective, and robust sorbents for the recovery of uranium from seawater. Here, we propose that the ligand design principles based on structural preorganization can be successfully applied to obtain a dramatic enhancement in UO 2 2+ ion binding affinity and selectivity. This concept is exemplified through the investigation of the com-plexes of UO 2 2+ , VO 2+ , and VO 2+ with the highly preorganized ligand PDA (1,10-phenanthroline-2,9-dicarboxylic acid) using a combination of fluores-cence and absorbance techniques, along with den-sity functional theory (DFT) calculations. Moreover, the measured stability constant value, log K1, of 16.5 for the UO 2 2+ /PDA complex is very high compared to uranyl complexes with other dicarboxylic ligands. Moreover, PDA exhibits strong selectivity for uranyl over vanadium ions, since the determined sta-bility constant values of the PDA complexes of the vanadium ions are quite low (V(IV) log K1 = 7.4, V(V) = 7.3). Finally, the structures of the corresponding UO 2 2+ , VO 2+ , and VO 2+ complexes with PDA were identified by systematic DFT calculations, and helped to interpret the stronger binding affinity for uranium over the vanadium ions. Due to its high chemical stability, selectivity, and structural preor-ganization for UO 2 2+ complexation, PDA is a very promising candidate that can be potentially used in the development of novel adsorbent materials for the selective extraction of uranium from sea-water.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials

Nuclear power is a relatively carbon-free energy source that has the capacity to be utilized today in an effort to stem the tides of global warming. The growing demand for nuclear energy, however, could put significant strain on our uranium ore resources, and the mining activities utilized to extract that ore can leave behind long-term environmental damage. A potential solution to enhance the supply of uranium fuel is to recover uranium from seawater using amidoximated adsorbent fibers. This technology has been studied for decades but is currently plagued by the material’s relatively poor selectivity of uranium over its main competitor vanadium. In this work, we investigate the binding schemes between uranium, vanadium, and the amidoxime functional groups on the adsorbent surface. Using quantum chemical methods, binding strengths are approximated for a set of complexation reactions between uranium and vanadium with amidoxime functionalities. Those approximations are then coupled with a comprehensive aqueous adsorption model developed in this work to simulate the adsorption of uranium and vanadium under laboratory conditions. Experimental adsorption studies with uranium and vanadium over a wide pH range are performed, and the data collected are compared against simulation results to validate the model. It was found that coupling ab initio calculations with process level adsorption modeling provides accurate predictions of the adsorption capacity and selectivity of the sorbent materials. Furthermore, this work demonstrates that this multiscale modeling paradigm could be utilized to aid in the selection of superior ligands or ligand compositions for the selective capture of metal ions. Furthermore, this first-principles integrated modeling approach opens the door to the in silico design of next-generation adsorbents with potentially superior efficiency and selectivity for uranium over vanadium in seawater.

36 MATERIALS SCIENCE↗

DOE OSTI2017

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

Amidoxime-functionalized polymeric adsorbents are the current state-of-the-art materials for collecting uranium (U) from seawater. However, marine tests show that vanadium (V) is preferentially extracted over U and many other cations. Here in this paper, we report a complementary and comprehensive investigation integrating ab initio simulations with thermochemical titrations and XAFS spectroscopy to understand the unusually strong and selective binding of V by polyamidoximes. While the open-chain amidoxime functionalities do not bind V, the cyclic imide-dioxime group of the adsorbent forms a peculiar non-oxido V 5+ complex, exhibiting the highest stability constant value ever observed for the V 5+ species. XAFS analysis of adsorbents following deployment in environmental seawater confirms V binding solely by the imide-dioximes. Our fundamental findings offer not only guidance for future optimization of selectivity in amidoxime-based sorbent materials, but may also afford insight to understanding the extensive accumulation of V in some marine organisms.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Multi-scale computer-aided design and photo-controlled macromolecular synthesis boosting uranium harvesting from seawater

By integrating multi-scale computational simulation with photo-regulated macromolecular synthesis, this study presents a new paradigm for smart design while customizing polymeric adsorbents for uranium harvesting from seawater. A dissipative particle dynamics (DPD) approach, combined with a molecular dynamics (MD) study, is performed to simulate the conformational dynamics and adsorption process of a model uranium grabber, i.e., PAO m -b-PPEGMA n , suggesting that the maximum adsorption capacity with atomic economy can be achieved with a preferred block ratio of 0.18. The designed polymers are synthesized using the PET-RAFT polymerization in a microfluidic platform, exhibiting a record high adsorption capacity of uranium (11.4 ± 1.2 mg/g) in real seawater within 28 days. This study offers an integrated perspective to quantitatively assess adsorption phenomena of polymers, bridging metal-ligand interactions at the molecular level with their spatial conformations at the mesoscopic level. The established protocol is generally adaptable for target-oriented development of more advanced polymers for broadened applications.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2012

Sonochemical functionalization of mesoporous carbon for uranium extraction from seawater

Extracting uranium from seawater is challenging due to its low concentration (3.3 ppb) and the myriad of competing ions. Mesoporous carbon materials provide a high surface area alternative to the traditional polymeric fiber braids developed for seawater extractions, specifically uranium extraction. In our work, sonochemical grafting of acrylonitrile onto the pores of soft-templated mesoporous carbons followed by its conversion to amidoxime functionalities was used to prepare an effective sorbent material with a high density of binding sites. Pore blockage, often observed for free radical polymerization, leads to poor adsorbent performance but can be easily overcome by the use of ultrasound during polymerization. Parameters such as surface area and surface pre-treatment, sonication intensity, solvent system, and monomer/initiator ratios were varied to optimize the polymerization and uranium adsorption capacity while not blocking the porosity, a significant hurdle in the utilization of functionalized porous materials. Our results show that neither the surface oxidation with nitric acid nor CO 2 activation alone is sufficient to cause significant improvement in grafting and uranium uptake. But, when coupled together, a greatly enhanced performance of the adsorbent materials was observed.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Low-cost desalination of seawater and hypersaline brine using nanophotonics enhanced solar energy membrane distillation

A stand-alone small-scale nanophotonics enhanced solar membrane distillation (NESMD) testbed was designed, developed, and tested for desalinating seawater and high salinity feedwaters. This NESMD system can take almost any source water and turn it into clean water with sunlight as the only energy source. The NESMD technology applies nanophotonic coating materials on a commercial hydrophobic polypropylene support of a polytetrafluoroethylene (PTFE) membrane surface. The photothermal coating serves as a solar thermal collector, absorbs solar energy, and generates highly localized heat on the membrane, while the rest of the membrane performs membrane distillation functions. The presented NESMD system is equipped with an internal heat recovery system with no need for external electricity and no additional water for cooling. The NESMD testbed is installed and tested at Rice University campus (29.7174° N, 95.4018° W). In this study, real seawater from Galveston Bay, Texas, U.S. and high salinity simulated feedwaters (total dissolved solids (TDS) of 113 200–200 000 PPM) have been tested for long-term testing under the weather conditions of Houston, Texas. Here, the field testing results showed stable desalination performance in consecutive 5–8 hour operation cycles, with a TDS removal of ≥99.5% in all experiments. An average daily membrane flux of ≥0.75 L m –2 h –1 was achieved at a solar intensity close to 1 kW m –2 without an external heat exchanger. Further investigations and improvements are required to enhance the performance of the reactor since it is still a new promising technology.

14 SOLAR ENERGY↗

DOE OSTI2013

The effects of total dissolved gas on chum salmon fry survival, growth, gas bubble disease, and seawater tolerance

Chum salmon Oncorhynchus keta alevin developing in gravel habitats downstream of Bonneville Dam on the Columbia River are exposed to elevated levels of total dissolved gas (TDG) when water is spilled at the dam to move migrating salmon smolts downstream to the Pacific Ocean. Current water quality criteria for the management of dissolved gas in dam tailwaters were developed primarily to protect salmonid smolts and are assumed to be protective of alevin if adequate depth compensation is provided. We studied whether chum salmon alevin exposed to six levels of dissolved gas ranging from 100% to 130% TDG at three development periods between hatch and emergence (hereafter early, middle, and late stage) suffered differential mortality, growth, gas bubble disease, or seawater tolerance. Each life stage was exposed for 50 d (early stage), 29 d (middle stage), or 16 d (late stage) beginning at 13, 34, and 37 d post-hatch, respectively, through 50% emergence. The mortality for all stages from exposure to emergence was estimated to be 8% (95% confidence interval (CI) of 4% to 12%) when dissolved gas levels were between 100% and 117% TDG. Mortality significantly increased as dissolved gas levels rose above 117% TDG,; with the lethal concentration that produced 50% mortality (LC50 ) was estimated to be 128.7% TDG (95% CI of 127.2% to 130.2% TDG) in the early and middle stages. By contrast, there was no evidence that dissolved gas level significantly affected growth in any life stage except that the mean wet weight at emergence of early stage fish exposed to 130% TDG was significantly less than the modeled growth of unexposed fish. The proportion of fish afflicted with gas bubble disease increased with increasing gas concentrations and occurred most commonly in the nares and gastrointestinal tract. Early stage fish exhibited higher ratios of filament to lamellar gill chloride cells than late stage fish, and these ratios increased and decreased for early and late stage fish, respectively, as gas levels increased; however, there were no significant differences in mortality between life stages after 96 h in seawater. The study results suggest that current water quality guidelines for the management of dissolved gas appear to offer a conservative level of protection to chum salmon alevin incubating in gravel habitat downstream of Bonneville Dam.

Geist, David R↗