Molecular-Level Modeling of Anode and Cathode Electrocatalysis for PEM Fuel Cells
Molecular-level modeling of heterogeneously catalyzed reactions is playing an increasingly important in the understanding of existing catalysts and the rational design of new catalysts. The progress in theoretical and computational modeling of heterogeneous catalysis, both in the gas and liquid phase, has been reviewed in several recent texts [1,2,3,4]. Although many of the conceptual aspects of modeling are similar, theoretical descriptions of catalytic reactions at the solid–liquid interface feature some important complications, mainly related to the presence of the liquid (electrolyte) phase and the electrical polarizability of the interface. This has consequences at various levels of theoretical and computational approaches.
The purpose of this chapter is to selectively summarize recent advances in the molecular modeling of anode and cathode electrocatalytic reactions employing different computational approaches, ranging from first-principlesquantum-chemical...
KeywordsDensity Functional Theory Oxygen Reduction Hollow Site Negative Field Solvent Reorganization
The work described in this chapter was done while I was at Eindhoven University of Technology. I would like to thank all my colleagues and co-authors who contributed to this work. Financial support from the Royal Netherlands Academy of Arts and Sciences (KNAW), the Netherlands Foundation for Scientific Research (NWO), and the Energy Research Centre of the Netherlands (ECN) and the European Union is also gratefully acknowledged.
- R.A. van Santen, M. Neurock, Catal. Rev. Sci. Eng. 37 357 (1995).Google Scholar
- M.T.M. Koper, R.A. van Santen, M. Neurock, in Catalysis and Electrocatalysis at Nanoparticle Surfaces, E.R. Savinova, C.G. Vayenas, A. Wieckowski, eds., Marcel Dekker, New York, p.1 (2003)Google Scholar
- F. Jensen, Introduction to Computational Chemistry, John Wiley & Sons, Chicester, (1999)Google Scholar
- M.T.M. Koper, in Modern Aspects of Electrochemistry, Eds. C.G. Vayenas, B.E. Conway, R.E. White, Kluwer Academic/Plenum Press, New York, Vol. 36, p. 51 (2003)Google Scholar
- M.P. Allen, D.J. Tildesley, Computer simulation of liquids, Clarendon, Oxford, (1987)Google Scholar
- D. Frenkel, B. Smit, Understanding Molecular Simulation, Academic Press, London, (2002)Google Scholar
- P.S. Bagus, C.J. Nelin, K. Hermann, M.R. Philpott, Phys. Rev. Lett. 36 8169 (1987)Google Scholar
- T. Ziegler, A. Rauk, Theor. Chim. Acta 46 1 (1977)Google Scholar
- C. Hartnig, E. Spohr, Chem. Phys. 319, 185 (2005)Google Scholar
- K. Kinoshita, Electrochemical Oxygen Technology, Wiley, New York, (1992)Google Scholar
- R.R. Adzic, in Electrocatalysis, Eds. J. Lipkowski,. P.N. Ross, Wiley, New York, p. 197 (1998)Google Scholar
- C. Hartnig, M.T.M. Koper, J. Electroanal. Chem. 531 165 (2002)Google Scholar
- P. Vassilev, M.T.M. Koper, J. Phys. Chem. C 111 2607 (2007)Google Scholar