First-principle Studies of Environmental Chemistry
EMSL Project ID
48872
Abstract
The overarching theme of this proposal is the study of chemical interactions in problems of environmental interest. We request supercomputing support from EMSL for two projects focusing on environmental chemistry that require quantum chemistry simulations. The scope of these two projects line up well with EMSL’s overall mission to predictively understand and accelerate solutions for national environmental challenges. It will also impact two of EMSL’s thrusts, on Terrestrial and Subsurface Ecosystems and Atmospheric Aerosol Systems. The first project is to study chemical reactivity of actinide complexes under hydrothermal conditions, that is, high-temperature and high-pressure situations. Ab-initio molecular dynamics studies will be used to extract the coordination environment of species under these extreme conditions, and to compute spectroscopic signatures that will allow us to validate the simulations with experimental probes. These conditions are found in geologically active regions or in the unfortunate situation of a nuclear accident as it happened in Japan in 2011. The second project is to study the sequestration of CO2 if flue gas. This project will use multiscale modeling in to develop new strategies to efficiently reduce atmospheric emission of CO2, the principal greenhouse gas linked to climate change. Though DOE/NETL is sponsoring several sorbent development efforts, significant effort is needed to understand the chemical nature and optimize the adsorption processes needed for successful sorbent capture systems. Both these project call for massive supercomputing support, one due to the high cost of hundred-atom ab-initio MD simulations. The other due to the requirement of high-level ab initio calculations are needed for this project to get accurate predictions of adsorption energies, kinetic barriers and diffusion mechanisms. Project Details
Project type
Large-Scale EMSL Research
Start Date
2015-10-01
End Date
2017-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Kelley M P,Yang P ,Clark S B,Clark A E 2016. "Structural and Thermodynamic Properties of the CmIII Ion Solvated by Water and Methanol" Inorganic Chemistry 55(10):4992–4999. 10.1021/acs.inorgchem.6b00477
Li WL, HT Liu, T Jian, GV Lopez, ZA Piazza, DL Huang, TT Chen, J Su, P Yang, X Chen, LS Wang, and J Li. 2015. "Bond-bending Isomerism of Au2I3?: Competition Between Covalent Bonding and Aurophilicity." Chemical Science 7:475-481. doi:10.1039/C5SC03568F
Winston M S,Batista E R,Yang P ,Tondreau A M,Boncella J M 2016. "Extending Stannyl Anion Chemistry to the Actinides: Synthesis and Characterization of a Uranium–Tin Bond" Inorganic Chemistry 55(11):5534–5539. 10.1021/acs.inorgchem.6b00543
Yeh YH ,Gorte R J,Rangarajan S ,Mavrikakis E 2016. "Adsorption of Small Alkanes on ZSM-5 Zeolites: Influence of Brønsted Sites" Journal of Physical Chemistry C 120(22):12132–12138. 10.1021/acs.jpcc.6b03855