451599 Modelling the Electrochemical Interface: Applications to CO2 Reduction

Wednesday, November 16, 2016: 10:05 AM
Franciscan D (Hilton San Francisco Union Square)
Karen Chan, Department of Chemical Engineering, SUNCAT Center for Interface Science and Catalysis, Stanford University and SLAC National Accelerator Laboratory, Stanford, CA; Stanford University

The electroreduction of CO2 has the potential to store energy from intermittent renewable sources and to produce carbon-neutral fuels and chemicals [1, 2]. In recent years, theoretical studies of CO2 reduction have usually applied the computational hydrogen electrode model, which allows for the determination of the energies of reaction intermediates without explicitly treating the potential and the ions in solution [3]. In this talk, I will first review the application of this approach to CO2 reduction: the determination of lowest free energy pathways and correlation of theoretical activity volcanoes with experimental onset potentials  [4, 5], and the computational screening of new catalysts [6].  I will then focus on recent developments in the explicit treatment of the electrochemical interface [7], required for an understanding of charge transfer barriers, kinetics, and selectivity.  I will discuss the scaling of CO2 reduction barriers,  field effects,  C-C coupling [8], and the integration of these effects into microkinetic models.

  1. Whipple, D. T. & Kenis, P. J. a. Prospects of CO 2 Utilization via Direct Heteroge- neous Electrochemical Reduction. J. Phys. Chem. Lett. 1, 3451–3458 (Dec. 2010).

  2. Graves, C., Ebbesen, S. D., Mogensen, M. & Lackner, K. S. Sustainable hydrocarbon fuels by recycling CO 2 and H 2 O with renewable or nuclear energy. Renewable and Sustainable Energy Reviews 15, 1–23 (2011).

  3. Nørskov, J. K., Rossmeisl, J., Logadottir, A., Lindqvist, L., Kitchin, J. R., Bligaard, T. & Jónsson, H. Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode. J. Phys. Chem. B 108, 17886–17892 (Nov. 2004).

  4. Shi, C., Hansen, H. a., Lausche, A. C. & Nørskov, J. K. Trends in electrochemical CO2 reduction activity for open and close-packed metal surfaces. Phys. Chem. Chem. Phys. 16, 4720–7 (Mar. 2014).

  5. Kuhl, K. P., Hatsukade, T., Cave, E. R., Abram, D. N., Kibsgaard, J. & Thomas, F. Electrocatalytic conversion of carbon dioxide to methane and methanol on transition metal surfaces (2014).

  6. Chan, K., Tsai, C., Hansen, H. A. & Nørskov, J. K. Molybdenum sulfides and selenides as possible electrocatalysts for CO2 reduction. ChemCatChem 6, 1899–1905 (2014).

  7. Chan, K. & Nørskov, J. K. Electrochemical Barriers Made Simple. J. Phys. Chem. Lett. 2663–2668 (2015).

  8. Montoya, J. H., Shi, C., Chan, K. & Nørskov, J. K. Theoretical Insights into a CO Dimerization Mechanism in CO2 Electroreduction. The journal of physical chemistry letters 6, 2032–2037 (2015). 


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See more of this Session: Computational Catalysis II: Electrocatalysis and Photocatalysis
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