Investigations into the Reusability of Amidoxime-Based Polymeric Adsorbents for Seawater Uranium Extraction

被引:46
作者
Kuo, Li-Jung [1 ]
Pan, Horng-Bin [2 ]
Wai, Chien M. [2 ]
Byers, Margaret F. [3 ]
Schneider, Erich [3 ]
Strivens, Jonathan E. [1 ]
Janke, Christopher J. [4 ]
Das, Sadananda [4 ]
Mayes, Richard T. [4 ]
Wood, Jordana R. [1 ]
Schlafer, Nicholas [1 ]
Gill, Gary A. [1 ]
机构
[1] Pacific Northwest Natl Lab, Marine Sci Lab, Sequim, WA 98382 USA
[2] Univ Idaho, Dept Chem, Moscow, ID 83844 USA
[3] Univ Texas Austin, Nucl & Radiat Engn Program, Austin, TX 78712 USA
[4] Oak Ridge Natl Lab, POB 2008, Oak Ridge, TN 37831 USA
关键词
SEQUESTERING URANIUM; RECOVERY; ELUTION; COST; PERFORMANCE; ADSORPTION; RADICALS;
D O I
10.1021/acs.iecr.7b02893
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
The ability to reuse amidoxime-based polymeric adsorbents is a critical component in reducing the overall cost of the technology to extract uranium from seawater. This report describes an evaluation of adsorbent reusability in multiple reuse (adsorption/stripping) cycles in. real seawater exposures with potassium bicarbonate (KHCO3) elution using several amidoxime-based polymeric adsorbents. The KHCO3 elution technique achieved similar to 100% recovery of uranium adsorption capacity in the first reuse. Subsequent reuses showed significant drops in adsorption capacity. After the fourth reuse with the ORNL AI8 adsorbent, the 56-day adsorption capacity dropped to 28% of its original capacity. FTIR spectra revealed that there was a conversion of the amidoxime ligands to carboxylate groups during extended seawater exposure, becoming more significant with longer exposure times. Ca and Mg adsorption capacities also increased with each reuse cycle supporting the hypothesis that long-term exposure resulted in converting amidoxime to carboxylate, enhancing the adsorption of Ca and Mg. Shorter seawater exposure (adsorption/stripping) cycles (28 vs 42 days) had higher adsorption capacities after reuse, but the shorter exposure cycle time did not produce an overall better performance in terms of cumulative exposure time. Recovery of uranium capacity in reuses may also vary across different adsorbent formulations. Through multiple reuses, the AI8 adsorbent can harvest 10 g uranium/kg adsorbent in similar to 140 days, using a 28-day adsorption/stripping cycle, a performance much better than would be achieved with a single use of the adsorbent through a very long-term exposure (saturation capacity of 7.4 g U/kg adsorbent). A time dependent seawater exposure model to evaluate the cost associated with reusing amidoxime-based adsorbents in real seawater exposures was developed. The predicted cost to extract uranium from seawater ranged from $610/kg U to $830/kg U. Model simulation suggests that a short seawater exposure cycle (<15 days) is the optimal deployment period for lower uranium production cost in seawater uranium mining.
引用
收藏
页码:11603 / 11611
页数:9
相关论文
共 30 条
[1]   Uranium Adsorbent Fibers Prepared by Atom-Transfer Radical Polymerization (ATRP) from Poly(vinyl chloride)-co-chlorinated Poly(vinyl chloride) (PVC-co-CPVC) Fiber [J].
Brown, Suree ;
Yue, Yanfeng ;
Kuo, Li-Jung ;
Mehio, Nada ;
Li, Meijun ;
Gill, Gary ;
Tsouris, Costas ;
Mayes, Richard T. ;
Saito, Tomonori ;
Dai, Sheng .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2016, 55 (15) :4139-4148
[2]   Optimization of the Passive Recovery of Uranium from Seawater [J].
Byers, M. Flicker ;
Schneider, E. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2016, 55 (15) :4351-4361
[3]   Novel poly(imide dioxime) sorbents: Development and testing for enhanced extraction of uranium from natural seawater [J].
Das, S. ;
Brown, S. ;
Mayes, R. T. ;
Janke, C. J. ;
Tsouris, C. ;
Kuo, L. -J. ;
Gill, G. ;
Dai, S. .
CHEMICAL ENGINEERING JOURNAL, 2016, 298 :125-135
[4]   Extracting Uranium from Seawater: Promising AF Series Adsorbents [J].
Das, S. ;
Oyola, Y. ;
Mayes, Richard T. ;
Janke, Chris J. ;
Kuo, L. -J. ;
Gill, G. ;
Wood, J. R. ;
Dai, S. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2016, 55 (15) :4110-4117
[5]  
Das S, 2016, IND ENG CHEM RES, V55, P4103, DOI 10.1021/acs.iecr.5b03135
[6]   RECOVERY OF URANIUM FROM SEAWATER .13. LONG-TERM STABILITY-TESTS FOR HIGH-PERFORMANCE CHELATING RESINS CONTAINING AMIDOXIME GROUPS AND EVALUATION OF ELUTION PROCESS [J].
EGAWA, H ;
KABAY, N ;
SHUTO, T ;
JYO, A .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1993, 32 (03) :540-547
[7]   Building future nuclear power fleets: The available uranium resources constraint [J].
Gabriel, Sophie ;
Baschwitz, Anne ;
Mathonniere, Gilles ;
Fizaine, Florian ;
Eleouet, Tommy .
RESOURCES POLICY, 2013, 38 (04) :458-469
[8]   The Uranium from Seawater Program at the Pacific Northwest National Laboratory: Overview of Marine Testing, Adsorbent Characterization, Adsorbent Durability, Adsorbent Toxicity, and Deployment Studies [J].
Gill, Gary A. ;
Kuo, Li-Jung ;
Janke, Chris J. ;
Park, Jiyeon ;
Jeters, Robert T. ;
Bonheyo, George T. ;
Pan, Horng-Bin ;
Wai, Chien ;
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, R. Shane ;
Chouyyok, Wilaiwan ;
Das, Sadananda ;
Kim, Jungseung ;
Buesseler, Ken ;
Breier, Crystal ;
D'Alessandro, Evan .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2016, 55 (15) :4264-4277
[9]  
Hall S., 2013, 20125239 USGS, P56
[10]   Cyclic Imide Dioximes: Formation and Hydrolytic Stability [J].
Kang, Sung Ok ;
Vukovic, Sinisa ;
Custelcean, Radu ;
Hay, Benjamin P. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2012, 51 (19) :6619-6624