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Title: The uranium from seawater program at PNNL: Overview of marine testing, adsorbent characterization, adsorbent durability, adsorbent toxicity, and deployment studies

The Pacific Northwest National Laboratory's (PNNL) Marine Science Laboratory (MSL) located along the coast of Washington State is evaluating the performance of uranium adsorption materials being developed for seawater extraction under realistic marine conditions with natural seawater. Two types of exposure systems were employed in this program: flow-through columns for testing of fixed beds of individual fibers and pellets and a recirculating water flume for testing of braided adsorbent material. Testing consists of measurements of the adsorption of uranium and other elements from seawater as a function of time, typically 42 to 56 day exposures, to determine the adsorbent capacity and adsorption rate (kinetics). Analysis of uranium and other trace elements collected by the adsorbents was conducted following strong acid digestion of the adsorbent with 50% aqua regia using either Inductively Coupled Plasma Optical Emission Spectrometry (ICP-OES) or Inductively Coupled Plasma Mass Spectrometer (ICP-MS). The ORNL 38H adsorbent had a 56 day adsorption capacity of 3.30 ± 0.68 g U/ kg adsorbent (normalized to a salinity of 35 psu), a saturation adsorption capacity of 4.89 ± 0.83 g U/kg of adsorbent material (normalized to a salinity of 35 psu) and a half-saturation time of 28 10 days. The AF1 adsorbentmore » material had a 56 day adsorption capacity of 3.9 ± 0.2 g U/kg adsorbent material (normalized to a salinity of 35 psu), a saturation capacity of 5.4 ± 0.2 g U/kg adsorbent material (normalized to a salinity of 35 psu) and a half saturation time of 23 2 days. The ORNL amidoxime-based adsorbent materials are not specific for uranium, but also adsorb other elements from seawater. The major doubly charged cations in seawater (Ca and Mg) account for a majority of the cations adsorbed (61% by mass and 74% by molar percent). For the ORNL AF1 adsorbent material, U is the 4th most abundant element adsorbed by mass and 7th most abundant by molar percentage. Marine testing at Woods Hole Oceanographic Institution with the ORNL AF1 adsorbent produced 15% and 55% higher adsorption capacities than observed at PNNL for column and flume testing, respectively. Variations in competing ions may be the explanation for the regional differences. In addition to marine testing, a number of other efforts are underway to characterize adsorbents and impacts of deployment on the marine environment. Highlights include: Hydrodynamic modelling predicts that a farm of adsorbent materials will likely have minimal effect on ocean currents and removal of uranium and other elements from seawater when densities are < 1800 braids/km2. A decrease in U adsorption capacity of up to 30% was observed after 42 days of exposure due to biofouling when the ORNL braided adsorbent AI8 was exposed to raw seawater in a flume in the presence of light. An identical raw seawater exposure with no light exposure showed little or no impact to adsorption capacity from biofouling. No toxicity was observed with column effluents of any absorbent materials tested to date. Toxicity could be induced with some non amidoxime-based absorbents only when the ratio of solid absorbent to test media was increased to highly unrealistic levels. Thermodynamic modeling of the seawater-amidoxime adsorbent was performed using the geochemical modeling program PHREEQC. Modeling of the binding of Ca, Mg, Fe, Ni, Cu, U, and V from batch interactions with seawater across a variety of concentrations of the amidoxime binding group reveal that when binding sites are limited (1 x 10-8 binding sites/kg seawater), vanadium heavily out-competes other ions for the amidoxime sites. In contrast, when binding sites are abundant magnesium and calcium dominate the total percentage of metals bound to the sorbent.« less
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [3] ;  [3] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [4] ;  [2] ;  [2] ;  [2] ;  [1] ;  [1] ;  [4] more »;  [4] ;  [2] ;  [2] ;  [5] ;  [5] ;  [6] « less
  1. Marine Sciences Lab., Sequim, WA (United States). Pacific Northwest National Lab.
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Idaho, Moscow, ID (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  5. Woods Hole Oceanographic Institution, Woods Hole, MA (United States)
  6. Univ. of Miami, Miami, FL (United States)
Publication Date:
OSTI Identifier:
1286943
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 55; Journal Issue: 15; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Nuclear Energy (NE)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE uranium; seawater; amidoxime; adsorption capacity; adsorption kinetics; marine testing; uranium toxicity; biofouling; themodynamic modelling