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Chemical Speciation of Americium, Curium, and Selected Tetravalent Actinides in High Level Waste (Felmy EMSP-tank, PNNL Scope #26753)


EMSL Project ID
4591

Abstract

Develop fundamental data on chemical speciation and solubility for Americium, Curium, and Selected Tetravalent Actinides in High Level Waste

Work authorization text added 08/11/05:
The objective of this project is to develop accurate chemical models to predict changes in HLW tank chemistry. We have completed our model for Sr complexation for the Hanford waste tanks, and the majority of the studies on chelate complexation of the trivalent actinides to high ionic strength. The experimental studies now focus on the tetravalent actinides. Interestingly, we have found that organic ligands adsorb to the solid phases at high base. This is somewhat surprising since it has been common wisdom that such adsorption of metal-chelate complexes should not occur in the presence of a negatively charged surface. If true, adsorption of such metal-chelate complexes could inhibit migration in the subsurface even under basic conditions. In addition, we also prepared another version of the "Felmy" database for use by site engineers using the ESP model. Dr. Felmy was also asked to serve as the Hanford site - EMSP HLW coordinator. Contact Andy Felmy, project manager, for additional information. Assumptions - The DOE client (Office of Biological and Environmental Research) expects us to conduct fundamental research to further our knowledge in areas of importance to DOE's mission, and to disseminate this knowledge through publications in peer-reviewed journals and presentations of results at scientific meetings. Products/Deliverables: - Publications in scientific journals - Presentations at scientific meetings and symposia.

Project Details

Project type
Exploratory Research
Start Date
2003-08-15
End Date
2006-03-27
Status
Closed

Team

Principal Investigator

Herman Cho
Institution
Pacific Northwest National Laboratory

Team Members

Zheming Wang
Institution
Pacific Northwest National Laboratory

Odeta Qafoku
Institution
Environmental Molecular Sciences Laboratory

Jean-Francois Boily
Institution
Umea University

Related Publications

Cao R, K Mushra, X Li, J Qian, MH Engelhard, ME Bowden, KS Han, KT Mueller, WA Henderson, and J Zhang. 2016. "Enabling room temperature sodium metal batteries." Nano Energy 30:825-830. doi:10.1016/j.nanoen.2016.09.013
Cao R, W Xu, D Lu, J Xiao, and J Zhang. 2015. "Anodes for Rechargeable Lithium-Sulfur Batteries." Advanced Energy Materials 5(16):Article No. 1402273. doi:10. 1002/aenm. 201402273
Deng X, MY Hu, X Wei, W Wang, Z Chen, J Liu, and JZ Hu. 2015. "Natural Abundance 17O NMR and Computational Modeling Studies of Lithium Based Liquid Electrolytes." Journal of the American Chemical Society 285(2015):146-155. doi:10.1016/j.jpowsour.2015.03.091
Felmy AR, and MJ Mason. 2003. "An Aqueous Thermodynamic Model for the Complexation of Sodium and Strontium with Organic Chelates valid to High Ionic Strength. I. Ethylenedinitrilotetraacetic acid (EDTA)." Journal of Solution Chemistry 32(4):283-300.
Felmy AR, and O Qafoku. 2004. "An Aqueous Thermodynamic Model for the Complexation of Nickel with EDTA Valid to high Base Concentration." Journal of Solution Chemistry 33(9):1161-1180.
Felmy AR, MJ Mason, and O Qafoku. 2003. "An Aqueous Thermodynamic Model for the Complexation of Sodium and Strontium with Organic Chelators valid to High Ionic Strength. II. N-(2-hydroxyethyl)ethylenedinitrilotriacetic acid (HEDTA)." Journal of Solution Chemistry 32(4):301-318.
Huang Q, ED Walter, L Cosimbescu, D Choi, and JP Lemmon. 2016. "In situ electrochemical-electron spin resonance investigations of multi-electron redox reaction for organic radical cathodes." Journal of Power Sources 306:812-816. doi:10. 1016/j. jpowsour. 2015. 11. 080
Hu JZ, Z Zhao, MY Hu, J Feng, X Deng, X Chen, W Xu, J Liu, and J Zhang. 2016. "In situ 7Li and 133Cs Nuclear Magnetic Resonance Investigations on the Role of Cs+ Additive in Lithium-Metal Deposition Process." Journal of Power Sources 304:51-59. doi:10.1016/j.jpowsour.2015.10.067
Kerisit SN, B Schwenzer, and M Vijayakumar. 2014. "Effects of Oxygen-Containing Functional Groups on Supercapacitor Performance." Journal of Physical Chemistry Letters 5(13):2330-2334. doi:10.1021/jz500900t
Kim YK, BD Kay, JM White, and Z Dohnalek. 2008. "2-Propanol Dehydration on TiO2(110): The Effect of Bridge-Bonded Oxygen Vacancy Blocking." Surface Science 602(2):511-516. doi:10.1016/j.susc.2007.10.049
Li G, X Lu, JY Kim, MH Engelhard, JP Lemmon, and VL Sprenkle. 2014. "The Role of FeS in Initial Activation and Performance Degradation of Na-NiCl2 (ZEBRA) Batteries ." PNNL-SA-101665, Pacific Northwest National Laboratory, Richland, WA. [Unpublished]
Liu J, J Zhang, Z Yang, JP Lemmon, CH Imhoff, GL Graff, L Li, JZ Hu, CM Wang, J Xiao, G Xia, VV Viswanathan, S Baskaran, VL Sprenkle, Y Shao, and B Schwenzer. 2012. "Materials Science and Materials Chemistry for Large Scale Electrochemical Energy Storage - From Transportation to Electrical Grid." Advanced Functional Materials. doi:10.1002/adfm.201200690
Qafoku O, and AR Felmy. 2007. "Development of Accurate Chemical Equilibrium Models for Oxalate Species to High Ionic Strength in the System: Na-Ba-Ca-Mn-Sr-Cl-NO3-PO4-SO4-H2O at 25?C." Journal of Solution Chemistry 36(1):81-95.
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Tang W, Y Liu, C Peng, MY Hu, X Deng, M Lin, JZ Hu, and KP Loh. 2015. "Probing Lithium Germanide Phase Evolution and Structural Change in a Germanium-in-Carbon Nanotube Energy Storage System." Journal of the American Chemical Society 137(7):2600-7. doi:10.1021/ja5116259
Vijayakumar M, BM Sivakumar, P Nachimuthu, B Schwenzer, S Kim, Z Yang, J Liu, GL Graff, S Thevuthasan, and JZ Hu. 2011. "Spectroscopic Investigations of the fouling process on Nafion membranes in vanadium redox flow Batteries." Journal of Membrane Science 366(1-2):325-334. doi:10.1016/j.memsci.2010.10.018
Vijayakumar M, B Schwenzer, S Kim, Z Yang, S Thevuthasan, J Liu, GL Graff, and JZ Hu. 2011. "Investigation of Local Environments in Nafion-SiO2 composite membranes used in Vanadium Redox Flow Battery." PNNL-SA-80357, Pacific Northwest National Laboratory, Richland, WA.
Vijayakumar M, B Schwenzer, V Shutthanandan, JZ Hu, J Liu, and IA Aksay. 2014. "Elucidating graphene - Ionic Liquid interfacial region: a combined experimental and computational study." Nano Energy 3:152-158. doi:10.1016/j.nanoen.2012.09.014
Vijayakumar M, L Li, GL Graff, J Liu, H Zhang, Z Yang, and JZ Hu. 2011. "Towards understanding the poor thermal stability of V5+ electrolyte solution in Vanadium Redox Flow Batteries." Journal of Power Sources 196(7):3669-3672. doi:10.1016/j.jpowsour.2010.11.126
Vijayakumar M, L Li, Z Nie, Z Yang, and JZ Hu. 2012. "Structure and Stability of Hexa-Aqua V(III) Cations in Vanadium Redox Flow Battery Electrolytes." Physical Chemistry Chemical Physics. PCCP 14(29):10233-10242. doi:10.1039/c2cp40707h
Vijayakumar M, N Govind, ED Walter, SD Burton, AK Shukla, A Devaraj, J Xiao, J Liu, CM Wang, AM Karim, and S Thevuthasan. 2014. "Molecular Structure and Stability of Dissolved Lithium Polysulfide Species." Physical Chemistry Chemical Physics. PCCP 16(22):10923-10932. doi:10.1039/c4cp00889H
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Vijayakumar M, SN Kerisit, KM Rosso, SD Burton, JA Sears, Jr, Z Yang, GL Graff, J Liu, and JZ Hu. 2011. "Lithium Diffusion in Li4Ti5O12 at High Temperatures." Journal of Power Sources 196(4):2211-2220.
Vijayakumar M, Z Nie, ED Walter, JZ Hu, J Liu, VL Sprenkle, and W Wang. 2015. "Understanding Aqueous Electrolyte Stability through Combined Computational and Magnetic Resonance Spectroscopy: A Case Study on Vanadium Redox Flow Battery Electrolytes." ChemPlusChem 80(2):428-437. doi:10.1002/cplu.201402139
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Zhang Z, RJ Rousseau, J Gong, SC Li, BD Kay, Q Ge, and Z Dohnalek. 2008. "Vacancy Assisted Diffusion of Alkoxy Species on Rutile TiO2(110)." Physical Review Letters 101(15):156103. doi:10.1103/PhysRevLett.101.156103
Zhao R, SJ Ding, Y Shen, DG Camp, II, EA Livesay, HR Udseth, and RD Smith. 2009. "Automated metal-free multiple-column nanoLC for improved phosphopeptide analysis sensitivity and throughput." Journal of Chromatography B 877(8-9):663-670.