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
Importance of Counteranions on the Hydration Structure of the Curium Ion
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
Free energies and mechanisms of water exchange around Uranyl from first principles molecular dynamics
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
Structure and Hydrolysis of the U(IV), U(V), and U(VI) Aqua Ions from Ab Initio Molecular Simulations
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