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Wet Chemical Synthesis of Atomically Precise Nanocatalysts

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Control of Structures on Complex Catalyst Supports

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Electrocatalytic Reduction of CO2

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Activation of CO on Metal Clusters

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Nano-structured Catalysts for CO Activation

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Modeling and Synthesis of Rare Earth Oxides

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Electrocatalytic Reduction of CO2
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Aravind Asthagiri Ulrike Diebold John Flake Greg Griffin Mike Janik Richard Kurtz Susan Sinnott James J Spivey Phil Sprunger

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PI names & Affiliations:

  • Aravind Asthagiri (Ohio State),
  • Ulrike Diebold (TU Vienna),
  • John Flake – Coordinator (LSU),
  • Greg Griffin (LSU),
  • Mike Janik (Penn. State),
  • Richard Kurtz (LSU),
  • Susan Sinnott (UF) ,
  • James J. Spivey (LSU),
  • Phil Sprunger (LSU).
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Objective: To understand CO2 reduction and develop the tools needed for designing electro catalysts are divided into three groups:
(1) Atomic-Level Simulation,
(2) Larger Time and Length Scale Simulation, and
(3) Experiment. The three groups work in close collaboration to bridge fundamental properties and practical behaviors using "cycles of learning".

Approach: Although empirical approaches to electrocatalyst development have yielded insight into one of the "grand challenges" in catalysis (CO2 conversion to valuable products like CH4 or CH3OH), reduction mechanisms are largely unknown. This project seeks to understand the electrocatalytic reduction of CO2 to alcohols at a fundamental level and developing the computational and experimental tools needed to create new electrocatalysts by design. This project is focused on extending the capabilities of first principles computational methods to more realistic length and time scales using charge optimized multi-body (COMB) potentials and adaptive kinetic Monte Carlo (akMC) simulations. These models are combined with surface-specific experiments (e.g. STM, TPD in-situ FTIR) to understand electrode behavior at an atomic level. Advancing the capabilities of computational simulation--from atomic scale to mm length scales; from 0 K and high vacuum conditions to room temperature and aqueous environments; and from ps to sec time scales—coupled with experimental validation of these models, represents a collaboration that would not occur without this EFRC.


Publications & Presentations:

1. M. Le, M. Ren, Z. Zhang, P. T. Sprunger, R. L. Kurtz, J. C. Flake, "Electrochemical Reduction of CO2 to CH3OH at Copper Oxide Surfaces", Journal of Electrochemical Society, 158(5), E45-E49, 2011.

2. T. A. Manz and D. S. Sholl "Methods for computing accurate atomic spin moments for collinear and noncollinear magnetism in periodic and nonperiodic materials", J. Chem. Theory Comput., J. Chem. Theory Comput., 2011, 7 (12), pp 4146–4164.

3. T.-R. Shan, B.D. Devine, J.M. Hawkins, A. Asthagiri, S.R. Phillpot, and S.B. Sinnott, "Second-generation charge-optimized many-body potential for Si/SiO2 and amorphous silica", Physical Review B 82, 235302 (2010).

4. J. Jansen, E. Lir, P. Galliker, J-G Wang, P. Sprunger, Z. Li, E. Laegsgaard, S. Wendt, B. hammer, F. Besenbacher, Enhancing Bonding of Silver Nanoparticles on Oxidized TiO2(110), J. Phys. Chem. C, 2010, 114 (40), pp 16964–16972.

5. J. Flake, "Electrocatalytic reduction of CO2 to CH3OH", Future Directions in CO2 Conversion Chemistry Workshop, Oct 2010, Princeton University.

6. M. Ren, M. Le, Z. Zhang, P. Sprunger, R. Kurtz, G. Griffin, and J. Flake, "Electrochemical Reduction of CO2 to Methanol at Copper Based Surfaces", Electrochemical Society Fall Meeting, Oct 2011, Boston, MA.

7. F. Wang, Z. Zhang, R.L. Kurtz, P.T. Sprunger, "Cu/Cu oxide growth on ZnO and TiO2 for CO2 reduction", APS, Mar 2011, Dallas, TX.

8. F. Womack, R. Singh, Y. Losovyi, O. Kizilkaya, R.L. Kurtz, P.T. Sprunger, "Electronic, Chemical, and Morphological Structure of Ag Nanoclusters grown on FeOx/Cu(100)", AVS, Oct 2010, Albuquerque, NM.

9. Z. Zhang, F. Wang, M. Le, M. Ren, J. Flake, P.T. Sprunger and R. L. Kurtz "Interaction of ZnO-supported Cu-oxides with CO and CO2: Electrochemical reduction of CO2 to CH3OH", AVS Oct 2011, Nashville, TN.

10. Z. Zhang, M. Ren, M. Le, M. Patterson, P.T. Sprunger, R. L. Kurtz, J. Flake, "Methanol synthesis on Cu-based catalyst: From amorphous Cu-oxide to O/Cu/Zn(1010)", Physical Electronics Conference, Jun 2010, University of Wisconsin – Milwaukee.

11. Z. Zhang, M. Patterson, M. Ren, Y. Losovyi, J. Flake, R.L. Kurtz, P.T. Sprunger, "Cu & CuOx Nanoclusters on ZnO(1010): Electronic, Catalytic, Morphological Structure", AVS, Oct 2010 Albuquerque, NM.

12. Z. Zhang, F. Wang, M. Ren, F. Womack, M. Le, Y. Losoyvi, R. Kurtz, P. Sprunger, J. Flake, "Cu/CuOx Nanoclusters on ZnO(1010): Catalytic, Structure and CO2 adsorption", APS March Meeting 2011, Dallas, TX.

13. MaomingRen, Le Minh, G. L. Griffin, and J.C. Flake, "Regenerative Methanol Fuel Cells: Reduction of CO2 to CH3OH on Oxidized Cu Electrodes" 218th ECS Meeting - Las Vegas, NV. 11/2010.

14. T.-R. Shan, B.D. Devine, T. Liang, S.R. Phillpot, S.B. Sinnott, "Charge optimized many body (COMB) potentials for complex systems", invited talk, Workshop on high fidelity 3D multiscale materials modeling and experimental analysis, Aug 2011.

15. T.-R. Shan, B.D. Devine, T. Liang, Y. Li, Y.-T. Cheng, S.R. Phillpot, S.B. Sinnott, "Charge optimized many body (COMB) potentials for complex systems", invited talk, 6th MIT Conference on Computational Fluid and Solid Mechanics, Jun 2011, Cambridge, MA.

16. R. Shan, B. Devine, T. Liang, Y. Li, Y.-T. Cheng, S.R. Phillpot, S.B. Sinnott, "Development and application of Charge-Optimized Many Body (COMB) potentials", invited talk, 5th meeting on Reactive Potential Development, Oct 2010, State College, PA.

17. T.-R. Shan, B.D. Devine, J. Yu, S.R. Phillpot, S.B. Sinnott, Classical Molecular dynamics simulations of heterogeneous interfacial systems with COMB potentials", invited talk, Center for Nanophase Materials Sciences Workshop, Sept 2010, Oak Ridge, TN.

18. Y.-T. Cheng, T.-R. Shan, T. Liang, B.D. Devine, B. Brooks-Hinojosa, S.R. Phillpot, A. Asthagiri, S.B. Sinnott, "Atomistic Simulations of the Adsorption and Mobility of Cu Adatoms on ZnO Surfaces using COMB Potentials", Surface Science (submitted 11/7/2011; revised 2/3/12).

19. S.B. Sinnott, "Charge Optimized Many-Body (COMB) Potentials", Workshop titled Materials Defects: Mathematics, Computation, and Engineering in Los Angeles, California, October 1-5, 2012.

20. S.B. Sinnott, "Charge Optimized Many-Body (COMB) Potentials: Development and Applications", Telluride Research Science Center Workshop titled Many-Body Interactions: From Quantum Mechanics to Force Fields in Telluride, Colorado, July 2-6, 2012.

21. S.B. Sinnott, "Molecular Dynamics Simulations of Polymer Surface Modification through Ion-Beam Deposition", Physical Chemistry Group, University of Helsinki in Helsinki, Finland, February 24, 2012.

22. S.B. Sinnott, "Charge Optimized Many-Body (COMB) Potentials for Interfacial Studies", Workshop titled Towards Reality in Nanoscale Materials in Levi, Finland, February 20-22, 2012.

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