Title: Enhancing uranium uptake by amidoxime adsorbent in seawater: An investigation for optimum alkaline conditioning parameters

Abstract

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 capacitymore » 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.« less

Authors:

Das, Sadananda ^[1]; Tsouris, Costas ^[1]; Zhang, Chenxi ^[1]; Brown, Suree ^[2]; Janke, Christopher James ^[1]; Mayes, Richard T. ^[1]; Kuo, Li -Jung ^[3]; Gill, Gary ^[3]; Dai, Sheng ^[4]; Kim, J. ^[1]; Oyola, Y. ^[2]; Wood, J. R. ^[3]

---

+ Show Author Affiliations

1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
2. Univ. of Tennessee, Knoxville, TN (United States)
3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:

Mon Sep 07 00:00:00 EDT 2015

Research Org.:

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:

USDOE Office of Nuclear Energy (NE)

OSTI Identifier:

1221730

Alternate Identifier(s):

OSTI ID: 1251638

Grant/Contract Number:  

AC05-00OR22725; AC05-76RL01830; AC05-76RL1830

Resource Type:

Accepted Manuscript

Journal Name:

Industrial and Engineering Chemistry Research

Additional Journal Information:

Journal Volume: 3; Journal Issue: 5; Journal ID: ISSN 0888-5885

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY