Reactivity and dynamics of complex systems
EMSL Project ID
47883
Abstract
The project involves an ongoing collaboration of 20+ researchers from University of Minnesota, University of South Carolina, Massachusetts Institute of Technology, and Pacific Northwest National Laboratory. The main goal of this project is to develop and apply innovative high-performance computing techniques and simulation methods for reactivity and dynamics of complex systems with special emphasis on the EMSL theme of the science of interfacial phenomena. The present proposal is concerned with application of advanced computational techniques to several fundamental fields of research including charge transport processes at interfaces, chemical and phase equilibria, thermochemical kinetics and rate constants, photochemistry, and spectroscopy. In particular, the proposal targets the following topics: (1) rational design of novel electrodes for solid oxide fuel cells, (2) nucleation and structure of aerosols, (3) metal-organic frameworks (MOFs) for adsorption, fractionation, and catalysis, (4) combustion mechanism of biofuels, and (5) spectroscopy of selected radical and ionic species in solution. The long-term goal of the first topic is to develop and apply more efficient computational methods and models for the design of complex oxide and metal-oxide surfaces and interfaces for high temperature electrochemical applications. In particular, we propose a computational study of the oxidation mechanism of hydrogen and natural gas and its reverse process, the reduction of water and carbon dioxide, on traditional nickel/yttria-stabilized-zirconia (Ni/YSZ) electrodes and novel electrodes based on doped perovskite crystals. The ultimate goal of the second topic is to better understand how liquid particles nucleate and grow in a multi-component gaseous mixture, and this is closely related to one area of the EMSL's current interest which is the formation and evolution of aerosol chemistry in the environment. We are interested in studying the formation of atmospheric sulfuric-acid-water-ammonia nanoparticles and nucleation phenomena in silane-based dusty plasmas. Our work on gaseous adsorption on MOFs includes alkanes, olefins, and oxygen molecules on Fe-MOF-74 and other MOFs with a similar structure. The purpose of this project is to study the ability of MOFs to adsorb and separate a mixture of gases which involves high costs and energy inputs when performed by currently used techniques such as cryogenic distillation and also study their catalytic properties. This work is being pursued in collaboration with U. S. Department of Energy Nanoporous Materials Genome Center (NMGC). Our computational study of the combustion mechanism of biofuels carried out in collaboration with U. S. Department of Energy Combustion Energy Frontier Research Center will eventually lead to developing predictive, multi-scale models with relevance to practical fuel combustion. Our work on the spectroscopy of selected radical and ionic species in solution will involve several species that are important intermediates in biological and environmental reductive chemistries of NO, and this work will be carried out in close collaboration with the pulse radiolysis lab at Brookhaven National Laboratory. Overall, the proposed work will eventually lead to more accurate and comprehensive computational models and protocols, and the design of such models and protocols will allow for handling new challenging problems in the future.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2015-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Ammal SC ,Heyden A 2014. "Water?Gas Shift Catalysis at Corner Atoms of Pt Clusters in Contact with a TiO2 (110) Support Surface" ACS Catalysis 4(10):3654–3662. 10.1021/cs5009706
Ammal SC ,Heyden A 2015. "Reaction Kinetics of the Electrochemical Oxidation of CO and Syngas Fuels on a Sr2Fe1.5Mo0.5O6?? Perovskite Anode" Journal of Materials Chemistry A 3(43):21618-21629. 10.1039/C5TA05056A
Aranifard S, SC Ammal, and A Heyden. 2014. "On the Importance of the Associative Carboxyl Mechanism for the Water-Gas Shift Reaction at Pt/CeO2 Interface Sites." Journal of Physical Chemistry C. doi:10.1021/jp5000649
Bender J D,Doraiswamy S ,Truhlar D G,Candler G V 2014. "Potential Energy Surface Fitting by a Statistically Localized, Permutationally Invariant, Local Interpolating Moving Least Squares Method for the Many-Body Potential: Method and Application to N4" Journal of Chemical Physics 140():054302. 10.1063/1.4862157
Faheem M ,Saleheen M ,Lu J ,Heyden A 2016. "Ethylene Glycol Reforming on Pt(111): First-principles Microkinetic Modeling in Vapor and Aqueous Phases" Catalysis Science & Technology 6(23):8242-8256. 10.1039/C6CY02111E
Huang, S.; Wilson, B. E.; Wang, B.; Fang, Y.; Buffington, K.; Stein, A.; Truhlar, D. G. ?Y-doped Li8ZrO6: A Li-Ion Battery Cathode Material with High Capacity?, J. Am. Chem. Soc. 2015, 137, 10992-11003.
Li, S. L.; Truhlar, D. G.; Schmidt, M. W.; Gordon, M. S. ?Model space diabatization for quantum photochemistry,? J. Chem. Phys. 2015, 142, 064106.
Li, S. L.; Xu, X.; Hoyer, C. E.; Truhlar, D. G. ?Nonintuitive Diabatic Potential Energy Surfaces for Thioanisole,? J. Phys. Chem. Lett. 2015, 6, 3352-3359.
Li, S. L.; Xu, X.; Truhlar, D. G. ?Computational simulation and interpretation of the low-lying excited electronic states and electronic spectrum of thioanisole,? Phys. Chem. Chem. Phys. 2015, 17, 20093-20099.
Mamun MO G,Walker E A,Faheem M ,Bond J Q,Heyden A 2017. "Theoretical Investigation of the Hydrodeoxygenation of Levulinic Acid to ?-Valerolactone over Ru(0001)" ACS Catalysis 7(1):215–228. 10.1021/acscatal.6b02548
Meana Paneda R, YY Paukku, K Duanmu, P Norman, D Schwartzenberger, and DG Truhlar. 2015. "Atomic Oxygen Recombination at Surface Defects on Reconstructed (0001) ?-Quartz Exposed to Atomic and Molecular Oxygen." Journal of Physical Chemistry C 119(17):9287–9301. doi:10.1021/acs.jpcc.5b00120
Paukku Y Y,Yang K ,Varga Z ,Truhlar D G 2014. "Erratum: “Global ab initio ground-state potential energy surface of N4”" Journal of Chemical Physics 140():019903. 10.1063/1.4861562
Shaikh N, M Valiev, and SV Lymar. 2014. "Decomposition of Amino Diazeniumdiolates (NONOates): Molecular Mechanisms ." Journal of Inorganic Biochemistry 141:28-35. doi:10.1016/j.jinorgbio.2014.08.008
Suthirakun S, SC Ammal, AB Munoz-Garcia, G Xiao, F Chen, HC zur Loye, EA Carter, and A Heyden. 2014. "Theoretical Investigation of H2 Oxidation on the Sr2Fe1. 5Mo0. 5O6 (001) Perovskite Surface Under Anodic Solid Oxide Fuel Cell Conditions." Journal of the American Chemical Society 136(23):8374–8386. doi:10. 1021/ja502629j
Varga Z, R Meana Paneda, G Song, YY Paukku, and DG Truhlar. 2016. "Potential energy surface of triplet N2O2." Journal of Chemical Physics 144(2):24310. doi:10.1063/1.4939008
Walker E A,Ammal SC ,Suthirakun S ,Chen F ,Terejanu G A,Heyden A 2014. "Mechanism of Sulfur Poisoning of Sr2Fe1.5Mo0.5O6-? Perovskite Anode" Journal of Physical Chemistry C 118(41):23545–23552. 10.1021/jp507593k
Walker E A,Ammal SC ,Terejanu G A,Heyden A 2016. "Uncertainty Quantification Framework Applied to the Water–Gas Shift Reaction over Pt-Based Catalysts" Journal of Physical Chemistry C 120(19):10328–10339. 10.1021/acs.jpcc.6b01348
Xu X, J Zheng, and DG Truhlar. 2015. "Ultraviolet Absorption Spectrum of Malonaldehyde in Water Is Dominated by Solvent-Stabilized Conformations." Journal of the American Chemical Society 137(25):8026–8029. doi:10.1021/jacs.5b04845