Large-scale computational modeling of the chemical transformation of actinide elements at interfaces
EMSL Project ID
44669
Abstract
Subsurface migration of radioactive waste resulting from nuclear energy and weapons production is a critical issue to the U.S. Department of Energy (DOE), and the safe and cost-effective disposal of this waste could be a limiting factor in deploying new energy technologies for the nation. Molecular-level processes, such as aqueous complexation, adsorption to, and the redox chemistry of actinide species in geochemical environments, often control the complex transport and reactive behavior of these species in chemically and physically heterogeneous subsurface environments. The ability to predict, control, or manipulate them is critical to virtually all aspects of environmental actinide chemistry.The goal of this project is to establish a fundamental and comprehensive molecular and multiscale understanding of the influence of complex real-world geochemical environments on the speciation, adsorption, reduction chemistry, and chemical transformation of actinide species, using to our advantage statistical and quantum mechanical computational chemistry tools and EMSL's supercomputing resources.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2011-10-01
End Date
2014-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Atta-Fynn R, DF Johnson, EJ Bylaska, ES Ilton, GK Schenter, and WA De Jong. 2012. "Structure and Hydrolysis of the U(IV), U(V), and U(VI) Aqua Ions from Ab Initio Molecular Simulations." Inorganic Chemistry 51(5):3016-3024. doi:10.1021/ic202338z
Atta-Fynn R, EJ Bylaska, and WA De Jong. 2012. "Free energies and mechanisms of water exchange around Uranyl from first principles molecular dynamics." In 2011 Materials Research Society Fall Meeting - Symposium A – Material Challenges in Current and Future Nuclear Technologies, vol. 1383, pp. mrsf11-1383-a07-06. Cambridge University Press, Cambridge, United Kingdom. doi:10.1557/opl.2012.181
Atta Fynn R, EJ Bylaska, and WA De Jong. 2013. "Importance of counteranions on the hydration structure of the curium ion." Journal of Physical Chemistry Letters 4(13):2166-2170. doi:10.1021/jz400887a
Gong Y, HS Hu, G Tian, L Rao, J Li, and JK Gibson. 2013. "A Tetrapositive Metal Ion in the Gas Phase: Thorium(IV) Coordinated by Neutral Tridentate Ligands." Angewandte Chemie International Edition 52(27):6885-6888. doi:10.1002/anie.201302212
Gong Y, WA De Jong, and JK Gibson. 2015. "Gas Phase Uranyl Activation: Formation of a Uranium Nitrosyl Complex from Uranyl Azide." Journal of the American Chemical Society 137(18):5911-5915. doi:10.1021/jacs.5b02420
Groenewold GS, MJ van Stipdonk, J Oomens, WA De Jong, and ME McIIwain. 2011. "The gas-phase bis-uranyl nitrate complex [(UO2)2(NO3)5]-: infrared spectrum and structure." International Journal of Mass Spectrometry 308(2-3):175-180. doi:10.1016/j.ijms.2011.06.002
Kuta J, MCF Wander, Z Wang, S Jiang, N Wall, and AE Clark. 2011. "Trends in Ln(III) Sorption to Quartz Assessed by Molecular Dynamics Simulations and Laser Induced Flourescence Studies." Journal of Physical Chemistry C 115(43):21120-21127. doi:10.1021/jp204633g
Kuta J, Z Wang, K Wisuri, MCF Wander, N Wall, and AE Clark. 2013. "The surface structure of ?-uranophane and its interaction with Eu(III) – An integrated computational and fluorescence spectroscopy study." Geochimica et Cosmochimica Acta 103:184-196. doi:10.1016/j.gca.2012.10.056
Odoh SO, and G Schreckenbach. 2013. "DFT Study of Uranyl Peroxo Complexes with H2O, F?, OH?, CO3 2?, and NO3?." Inorganic Chemistry 52(9):5590-5602. doi:10.1021/ic400652b
Odoh SO, EJ Bylaska, and WA De Jong. 2013. "Coordination and Hydrolysis of Plutonium Ions in Aqueous Solution using Car-Parrinello Molecular Dynamics Free Energy Simulations." Journal of Physical Chemistry A 117(47):12256-12267. doi:10.1021/jp4096248
Odoh SO, N Govind, G Schreckenbach, and WA De Jong. 2013. "Cation-Cation Interactions in [(UO2)2(OH)n](4-n) Complexes." Inorganic Chemistry 52(19):11269-11279. doi:10.1021/ic4015338
Parmar P, KA Peterson, and AE Clark. 2013. "Static Electric Dipole Polarizabilities of Tri- and Tetravalent U, Np, and Pu Ions." Journal of Physical Chemistry A 117(46):11874–11880. doi:10.1021/jp403078j
Rios D, GE Schoendorff, MJ Van Stipdonk, MS Gordon, TL Windus, JK Gibson, and WA De Jong. 2012. "Roles of Acetone and Diacetone Alcohol in Coordination and Dissociation Reactions of Uranyl Complexes." Inorganic Chemistry 51(23):12768-12775.
Samuels AC, CA Boele, KT Bennett, SB Clark, N Wall, and AE Clark. 2014. "Integrated Computational and Experimental Protocol for Understanding Rh(III) Speciation in Hydrochloric and Nitric Acid Solutions." Inorganic Chemistry 53(23):12315–12322. doi:10.1021/ic501408r
Tecmer P, N Govind, K Kowalski, WA De Jong, and L Visscher. 2013. "Reliable Modeling of the Electronic Spectra of Realistic Uranium Complexes." Journal of Chemical Physics 139(3):034301-1 to 034301-12.