Adsorbent Alkali Conditioning For Uranium Adsorption From Seawater Adsorbent Performance And Technology Cost Evaluation PDF Download

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Adsorbent Alkali Conditioning for Uranium Adsorption from Seawater. Adsorbent Performance and Technology Cost Evaluation

Adsorbent Alkali Conditioning for Uranium Adsorption from Seawater. Adsorbent Performance and Technology Cost Evaluation
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Total Pages: 41
Release: 2015
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The Fuel Resources program of the Fuel Cycle Research and Development program of the Office of Nuclear Energy (NE) is focused on identifying and implementing actions to assure that nuclear fuel resources are available in the United States. An immense source of uranium is seawater, which contains an estimated amount of 4.5 billion tonnes of dissolved uranium. This unconventional resource can provide a price cap and ensure centuries of uranium supply for future nuclear energy production. NE initiated a multidisciplinary program with participants from national laboratories, universities, and research institutes to enable technical breakthroughs related to uranium recovery from seawater. The goal is to develop advanced adsorbents to reduce the seawater uranium recovery technology cost and uncertainties. Under this program, Oak Ridge National Laboratory (ORNL) has developed a new amidoxime-based adsorbent of high surface area, which tripled the uranium capacity of leading Japanese adsorbents. Parallel efforts have been focused on the optimization of the physicochemical and operating parameters used during the preparation of the adsorbent for deployment. A set of parameters that need to be optimized are related to the conditioning of the adsorbent with alkali solution, which is necessary prior to adsorbent deployment. Previous work indicated that alkali-conditioning parameters significantly affect the adsorbent performance. Initiated in 2014, this study had as a goal to determine optimal parameters such as base type and concentration, temperature, and duration of conditioning that maximize the uranium adsorption performance of amidoxime functionalized adsorbent, while keeping the cost of uranium production low. After base-treatment at various conditions, samples of adsorbent developed at ORNL were tested in this study with batch simulated seawater solution of 8-ppm uranium concentration, batch seawater spiked with uranium nitrate at 75-100 ppb uranium, and continuous-flow natural seawater at the Pacific Northwest National Laboratory (PNNL). Fourier Transform Infrared (FTIR) spectroscopy, Nuclear Magnetic Resonance (NMR) spectroscopy, Scanning Electron Microscopy (SEM), and elemental analysis were used to characterize the adsorbent at different stages of adsorbent preparation and treatment. The study can be divided into two parts: (A) investigation of optimal parameters for KOH adsorbent conditioning and (B) investigation of other possible agents for alkali conditioning, including cost analysis on the basis of uranium production. In the first part of the study, tests with simulated seawater containing 8 ppm uranium showed that the uranium adsorption capacity increased with an increase in the KOH concentration and conditioning time and temperature at each of the KOH concentrations used. FTIR and solid state NMR studies indicated that KOH conditioning converts the amidoxime functional groups into more hydrophilic carboxylate. The longer the KOH conditioning time, up to three hours, the higher was the loading capacity from the simulated seawater solution which is composed of only uranyl, sodium, chloride, and carbonate ions. Marine testing with natural seawater, on the other hand, showed that the uranium adsorption capacity of the adsorbent increased with KOH conditioning temperature, and gradually decreased with increasing KOH conditioning time from one hour to three hours at 80 C. This behavior is due to the conversion of amidoxime to carboxylate. The carboxylate groups are needed to increase the hydrophilicity of the adsorbent; however, conversion of a significant amount of amidoxime to carboxylate leads to loss in selectivity toward uranyl ions. Thus, there is an optimum KOH conditioning time for each temperature at which an optimum ratio between amidoxime and carboxylate is reached. For the case of base conditioning with 0.44 M KOH at 80 C, the optimal conditioning time is 1 hour, with respect to the highest uranium loading capa ...

Alternative Alkaline Conditioning of Amidoxime Based Adsorbent for Uranium Extraction from Seawater

Alternative Alkaline Conditioning of Amidoxime Based Adsorbent for Uranium Extraction from Seawater
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Total Pages: 11
Release: 2015
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Alkaline conditioning of the amidoxime based adsorbents is a significant step in the preparation of the adsorbent for uranium uptake from seawater. The effects of various alkaline conditioning parameters such as the type of alkaline reagent, reaction temperature, and reaction time were investigated with respect to uranium adsorption capacity from simulated seawater (spiked with 8 ppm uranium) and natural seawater (from Sequim Bay, WA). An adsorbent (AF1) was prepared at the Oak Ridge National Laboratory by radiation-induced graft polymerization (RIGP) with acrylonitrile and itaconic acid onto high-surface-area polyethylene fibers. For the AF1 adsorbent, sodium hydroxide emerged as a better reagent for alkaline conditioning over potassium hydroxide, which has typically been used in previous studies, because of higher uranium uptake capacity and lower cost over the other candidate alkaline reagents investigated in this study. Furthermore, the use of sodium hydroxide in place of potassium hydroxide is shown to result in a 21-30% decrease in the cost of uranium recovery.

M4FT-15OR03100421

M4FT-15OR03100421
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Total Pages: 25
Release: 2015
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Significant progress in understanding the role of alkaline conditioning of polyethylene-fiber adsorbent, developed at the Oak Ridge National Laboratory (ORNL), is demonstrated in this report, which is essentially a manuscript prepared for publication in the journal Industrial and Engineering Chemistry Research of the American Chemical Society. The manuscript describes the influence of various parameters involved in adsorbent alkaline conditioning, including base concentration and duration and temperature of conditioning, on the uranium uptake history by the adsorbent. Various solutions have been used to determine the influence of conditioning parameters including (i) a screening solution containing uranyl nitrate at approximately 8 ppm and sodium bicarbonate and sodium chloride at concentrations similar to those found in seawater, (ii) seawater spiked with approximately 75 ppb uranium, and (iii) natural seawater. In addition to concentration measurements by inductively coupled plasma (ICP) spectroscopy to determine the uranium uptake capacity and kinetics, spectroscopic methods such as Fourier transformed infrared (FTIR) spectroscopy and nuclear magnetic resonance (NMR) spectroscopy were employed to investigate the effect of base treatment on the various chemical bonds of the adsorbent. Scanning electron microscopy (SEM) has also been employed to determine structural effects of the alkali on the adsorbent. The results are summarized as follows: 1. Alkali conditioning is necessary to prepare the adsorbent for uranium uptake. ICP analysis showed that without alkali conditioning, no appreciable uranium adsorption occurs. 2. FTIR showed that the base converts amidoxime to carboxylate groups. 3. FTIR showed that formation of carboxylate groups is irreversible and reduces the selectivity of the adsorbent toward uranium. 4. NMR showed that alkali conditioning leads also to the formation of cyclic imidedioxime, which is suspected to bind uranium, vanadium, iron, copper, and other metals. 5. Uptake of V, Fe, and Cu follows the same trend as that of uranium. Uptake of Ca, Mg, and Zn ions increases with increasing KOH conditioning time due to formation of carboxylate groups. 6. SEM showed that long conditioning times may also lead to adsorbent degradation. 7. The optimal conditioning parameters are: 0.44 M KOH, 70 C, for 1 hour. The results of this study are useful in the selection of optimal values of the parameters involved in preparing amidoxime-based adsorbent for uranium uptake from seawater. Additional work is still ongoing to provide a complete understanding of the chemistry of base conditioning and its role on the functioning of the adsorbent.

Uranium Extraction from Seawater

Uranium Extraction from Seawater
Author: Darshan Jitendra Sachde
Publisher:
Total Pages: 482
Release: 2011
Genre:
ISBN:
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Technology to recover uranium from seawater may act as a potential backstop on the production cost of uranium in a growing international nuclear industry. Convincing proof of the existence of an effective expected upper limit on the resource price would have a strong effect on decisions relating to deployment of uranium resource consuming reactor technologies. This evaluation proceeds from a review of backstop technologies to detailed analyses of the production cost of uranium extraction via an amidoxime braid adsorbent system developed by the Japan Atomic Energy Agency (JAEA). An independent cost assessment of the braid adsorbent system is developed to reflect a project implemented in the United States. The cost assessment is evaluated as a life cycle discounted cash flow model to account for the time value of money and time-dependent performance parameters. In addition, the cost assessment includes uncertainty propagation to provide a probabilistic range of uranium production costs for the braid adsorbent system. Results reveal that uncertainty in adsorbent performance (specifically, adsorption capacity, kg U/tonne adsorbent) is the dominant contributor to overall uncertainty in uranium production costs. Further sensitivity analyses reveal adsorbent capacity, degradation and production costs as key system cost drivers. Optimization of adsorbent performance via alternate production or elution pathways provides an opportunity to significantly reduce uranium production costs. Finally, quantification of uncertainty in production costs is a primary policy objective of the analysis. Continuing investment in this technology as a viable backstop requires the ability to assess cost and benefits while incorporating risk.

Investigations Into the Reusability of Amidoxime-Based Polymeric Uranium Adsorbents

Investigations Into the Reusability of Amidoxime-Based Polymeric Uranium Adsorbents
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Total Pages: 39
Release: 2016
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Significant advancements in amidoxime-based polymeric adsorbents to extract uranium from seawater are achieved in recent years. The success of uranium adsorbent development can help provide a sustainable supply of fuel for nuclear reactors. To bring down the production cost of this new technology, in addition to the development of novel adsorbents with high uranium capacity and manufacture cost, the development of adsorbent re-using technique is critical because it can further reduce the cost of the adsorbent manufacture. In our last report, the use of high concentrations of bicarbonate solution (3M KHCO3) was identified as a cost-effective, environmental friendly method to strip uranium from amidoxime-based polymeric adsorbents. This study aims to further improve the method for high recovery of uranium capacity in re-uses and to evaluate the performance of adsorbents after multiple re-use cycles. Adsorption of dissolved organic matter (DOM) on the uranium adsorbents during seawater exposure can hinder the uranium adsorption and slow down the adsorption rate. An additional NaOH rinse (0.5 M NaOH, room temperature) was applied after the 3 M KHCO3 elution to remove natural organic matter from adsorbents. The combination of 3 M KHCO3 elution and 0.5 M NaOH rinse significantly improves the recovery of uranium adsorption capacity in the re-used adsorbents. In the first re-use, most ORNL adsorbents tested achieve ~100% recovery by using 3 M KHCO3 elution + 0.5 M NaOH rinse approach, in comparison to 54% recovery when only 3 M KHCO3 elution was applied. A significant drop in capacity was observed when the adsorbents went through more than one re-use. FTIR spectra revealed that degradation of amidoxime ligands occurs during seawater exposure, and is more significant the longer the exposure time. Significantly elevated ratios of Ca/U and Mg/U in re-used adsorbents support the decrease in abundance of amidoxime ligands and increase carboxylate group from FT-IR analysis. The impact of the length of seawater exposure cycle in adsorbent re-use was evaluated by comparing the adsorption capacity for a common adsorbent formulation (ORNL AI8 formulation) under different exposure cycle (28 days and 42 days). Adsorbents with a 28 days seawater exposure cycle had higher recovery of uranium capacity than adsorbent with 42 days of seawater exposure. Under different cumulative seawater exposure time, the adsorbent with 28 days seawater exposure cycle also had less amidoxime ligands degradation than the adsorbent with 42 days seawater exposure cycle. These observations support the negative impact of prolonged seawater exposure on amidoxime ligands stability. Recovery of uranium capacity in re-uses also varies across different adsorbent formulations. Among three different ORNL adsorbents tested (AI8, AF8, AF1-DMSO), AI8 had the best recovery in each re-use, followed by AF8 and then AF1-DMSO. This demonstrates that continuing efforts on developing new adsorbents with high capacity and stability is critical. The overall performance of adsorbents in multiple re-use cycles can be evaluated by calculation total harvestable uranium, the summation of adsorbed uranium from each seawater exposure cycle. In this assessment, the ORNL AI8 braid with 28 days seawater exposure cycle can reach total harvestable uranium 10g Uranium/kg adsorbent in ~140 days; while the same type of braid but with 42 days seawater exposure cycle reach the same level in ~170 days. Notably, the performance of total harvestable uranium also varies among different adsorbent formulations (AI8> AF1-DMSO> AF8). Short seawater exposure cycle is associated with high re-use frequency. The development of low-cost offshore adsorbent deployment/extraction is essential for high frequency reuse operation. This study also highlights the importance to examine the re-use performance of newly developed uranium adsorbents for selection of optimal adsorbents for ocean deployment.

Graphene-Based Materials as Adsorbents for Wastewater Decontamination

Graphene-Based Materials as Adsorbents for Wastewater Decontamination
Author: Suprakas Sinha Ray
Publisher: CRC Press
Total Pages: 340
Release: 2024-10-07
Genre: Technology & Engineering
ISBN: 1040130445
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This book aims to provide a fundamental grasp of graphene-based materials (GAMs) and their adsorption process. The effect of diverse process parameters, including pH, temperature, agitation, competing ions, etc., on the adsorption performance of GAMs as well as their recent and relevant applications in biomedical fields, are discussed. The current challenges and future outlook have been addressed as an independent chapter, and the recyclability of these adsorbent materials has also been covered. Features: Focuses on graphene-based materials as adsorbents to remove contaminants from wastewater. Includes detailed computational and statistical analyses and cost comparison points. Compares the performance of graphene-based materials as adsorbents in the context of various other reported adsorbents, including other 2D materials, such as WS2 and BN. Provides fundamental comprehension of the graphene-based materials’ adsorption process. Discusses the recyclable nature of graphene-based materials, as well as approaches used. This book has been aimed at graduate students and researchers in wastewater treatment, environmental, materials, and chemical engineering.

Extracting Uranium from Seawater

Extracting Uranium from Seawater
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Release: 2015
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A series of adsorbent (AI10 through AI17) were successfully developed at ORNL by radiation induced graft polymerization (RIGP) of acrylonitrile (AN) and vinylphosphonic acid (VPA) (at different mole/mole ratios) onto high surface area polyethylene fiber, with higher degree of grafting which ranges from 110 300%. The grafted nitrile groups were converted to amidoxime groups by reaction with 10 wt% hydroxylamine at 80 C for 72 hours. The amidoximated adsorbents were then conditioned with 0.44M KOH at 80 C followed by screening at ORNL with simulated seawater spiked with 8 ppm uranium. Uranium adsorption capacity in simulated seawater screening ranged from 171-187 g-U/kg-ads irrespective of %DOG. The performance of the adsorbents for uranium adsorption in natural seawater was also carried out using flow-through-column at Pacific Northwest National Laboratory (PNNL). The three hours KOH conditioning was better for higher uranium uptake than one hour. The adsorbent AI11 containing AN and VPA at the mole ration of 3.52, emerged as the potential candidate for higher uranium adsorption (3.35 g-U/Kg-ads.) after 56 days of exposure in the seawater in the flow-through-column. The rate vanadium adsorption over uranium was linearly increased throughout the 56 days exposure. The total vanadium uptake was ~5 times over uranium after 56 days.

Enhancing Uranium Uptake by Amidoxime Adsorbent in Seawater

Enhancing Uranium Uptake by Amidoxime Adsorbent in Seawater
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Total Pages: 9
Release: 2015
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A high-surface-area polyethylene-fiber adsorbent (AF160-2) has been developed at the Oak Ridge National Laboratory by radiation-induced graft polymerization of acrylonitrile and itaconic acid. The grafted nitriles were converted to amidoxime groups by treating with hydroxylamine. The amidoximated adsorbents were then conditioned with potassium hydroxide (KOH) by varying different reaction parameters such as KOH concentration (0.2, 0.44, and 0.6 M), duration (1, 2, and 3 h), and temperature (60, 70, and 80 °C). Adsorbent screening was then performed with simulated seawater solutions containing sodium chloride and sodium bicarbonate, at concentrations found in seawater, and uranium nitrate at a uranium concentration of ~7-8 ppm and pH 8. Fourier transform infrared spectroscopy and solid-state NMR analyses indicated that a fraction of amidoxime groups was hydrolyzed to carboxylate during KOH conditioning. The uranium adsorption capacity in the simulated seawater screening solution gradually increased with conditioning time and temperature for all KOH concentrations. It was also observed that the adsorption capacity increased with an increase in concentration of KOH for all the conditioning times and temperatures. AF160-2 adsorbent samples were also tested with natural seawater using flow-through experiments to determine uranium adsorption capacity with varying KOH conditioning time and temperature. Based on uranium loading capacity values of several AF160-2 samples, it was observed that changing KOH conditioning time from 3 to 1 h at 60, 70, and 80 °C resulted in an increase of the uranium loading capacity in seawater, which did not follow the trend found in laboratory screening with stimulated solutions. Longer KOH conditioning times lead to significantly higher uptake of divalent metal ions, such as calcium and magnesium, which is a result of amidoxime conversion into less selective carboxylate. Lastly, scanning electron microscopy showed that long conditioning times may also lead to adsorbent degradation.

A Cost Estimate for Uranium Recovery from Seawater Using a Chitin Nanomat Adsorbent

A Cost Estimate for Uranium Recovery from Seawater Using a Chitin Nanomat Adsorbent
Author: Harry Dreyfus Lindner
Publisher:
Total Pages: 142
Release: 2014
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ISBN:
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Even at 3.3 ppb, seawater contains a uranium supply large enough to power the world's nuclear fleet for 13,000 years. This large supply has prompted interest in technologies for recovering uranium from seawater. Since the 1960's, economic models of such technologies have failed to produce an economically competitive strategy when compared to conventional uranium recovery from terrestrial mining. Thus, uranium from seawater is researched as a potential price ceiling because of the large supply but high recovery cost. Such an upper bound is still valuable research because it allows for more certainty in uranium prices for planning, research, development and deployment of nuclear power systems. This thesis explores past cost estimates for uranium recovery from seawater and adds a new cost estimate to the pool of literature. The past estimates showed a development from systems that actively moved seawater to systems that allowed adsorbent to sit passively in seawater. The adsorbent material changed from hydrous titanium oxide to the higher-capacity amidoxime ligand. Capacity was the strongest driver of cost. Early models with the amidoxime ligand used an acrylic substrate or backbone. This substrate was later replaced by polyethylene because of its increased durability and lower cost. However, each of those materials could contribute to the problem of plastics in the ocean. The new technology assessed for cost in this paper attempts to address the plastics concern by replacing the plastic with a high molecular weight chitin nanomat as the substrate for the amidoxime ligand. The cost assessment showed the technology is presently cost prohibitive largely due to the adsorption capacity and chitin nanomat production costs. To increase capacity, the grafting efficiency onto the chitin substrate must be improved in order to achieve capacities comparable to those observed for the amidoxime-polyethylene adsorbent. To reduce chitin nanomat production costs, the ionic liquid (IL) consumption must be reduced and the recyclability of IL must be achieved.

Determination of Adsorption Capacity and Kinetics of Amidoxime-Based Uranium Adsorbent Braided Material in Unfiltered Seawater Using a Flume Exposure System

Determination of Adsorption Capacity and Kinetics of Amidoxime-Based Uranium Adsorbent Braided Material in Unfiltered Seawater Using a Flume Exposure System
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Total Pages: 27
Release: 2015
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PNNL has developed a recirculating flume system for exposing braided adsorbent material to natural seawater under realistic temperature and flow-rate exposure conditions. The flumes are constructed of transparent acrylic material they allow external light to pass into the flumes and permit photosynthetic growth of naturally present marine organisms (biofouling). Because the system consists of two flumes, replicate experiments can be conducted in which one of the flumes can be manipulated relative to the other. For example, one flume can be darkened to eliminate light exposure by placing a black tarp over the flume such that dark/light experiments can be conducted. Alternatively, two different braided adsorbents can be exposed simultaneously with no potential cross contamination issues. This report describes the first use of the PNNL flume system to study the impact of biofouling on adsorbent capacity. Experiments were conducted with the ORNL AI8 braided adsorbent material in light exposed and darkened flumes for a 42 day exposure experiment. The major objective of this effort is to develop a system for the exposure of braided adsorbent material to unfiltered seawater and to demonstrate the system by evaluating the performance of adsorption material when it is exposed to natural marine biofouling as it would be when the technology is used in the marine environment. Exposures of amidoxime-based polymeric braid adsorbents prepared by Oak Ridge Natural Laboratory (ORNL) were exposed to ambient seawater at 20°C in a flume system. Adsorption kinetics and adsorption capacity were assessed using time series determinations of uranium adsorption and one-site ligand saturation modeling.