Dresden 2014 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 30: Surface Chemical Reactions and Heterogeneous Catalysis II

O 30.4: Vortrag

Dienstag, 1. April 2014, 11:15–11:30, PHY C 213

Photo-catalytic water splitting with co-catalysts: beyond proton-coupled electron transfer — •Harald Oberhofer, Markus Sinstein, Ran Jia, and Karsten Reuter — Technische Universität München, Germany

Efficient, sustainable production of molecular hydrogen—a promising alternative to batteries in terms of energy storage—is still an unsolved problem. Recently, we presented [1] a novel screening method for viable combinations of photocatalysts and metal co-catalysts based on the computational hydrogen electrode approach pioneered by Nørskov and Rossmeisl.[2] In this thermodynamic approach charge-neutral proton-coupled electron transfer (PCET) pathways are generally assumed. Any screening approach resting on this assumption may therefore falsely rule out viable catalysts following other, uncoupled pathways.

Using an implicit solvent model we recently implemented into the FHI-aims DFT package,[3] we extend our screening scheme to uncoupled reaction paths, where due to the occurrence of charged intermediates solvent screening effects can no longer be neglected. We present first results of our screening efforts and show that even for charge-neutral PCET pathways solvent effects can not be neglected. [1] H. Oberhofer, K. Reuter, J. Chem. Phys. 139, 44710 (2013).
[2] A. Valdes et al., J. Phys. Chem. C 112, 9872 (2008).
[3] V. Blum et al., Comp. Phys. Commun. 180, 2175 (2009).