Dresden 2017 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 107: Heterogeneous Catalysis: Theory II

O 107.3: Vortrag

Freitag, 24. März 2017, 11:00–11:15, TRE Phy

DFT modeling of formic acid decomposition over late transition metals: on the road to lower activation barriers — •Jan Kučera and Axel Groß — Institute of Theoretical Chemistry, Ulm University, D-89069 Ulm/Germany

Low temperature decomposition of formic acid (FA) to regain pure H₂ is among the processes suggested as one of the potential H₂-storage alternatives to designs employing compressed hydrogen. Heterogeneous catalysts based on late transition metals, in particular Pd or Au particles dispersed on oxide supports, selectively decompose formic acid already at low temperatures, however, so far the achieved efficiencies are below those required for commercial polymer electrolyte membrane fuel cells.

The general goal of our computational study - based mainly on periodical density functional theory (DFT) calculations - relates to the identification of the key effects operating in FA decomposition at Pd and Au-based surfaces and at complex metal/oxide interfaces. Despite the fact that in principle only two dehydrogenation steps are involved, FA decomposition represents a complex catalytic system. We will focus on the elucidation of three phenomena that might be critical for the reaction energetics: (i) modification of catalytic properties by the formation of bimetallic surfaces, (ii) the role of intermolecular forces in the formate decomposition step due to dimer configurations or the interaction with the solvent, and (iii) the effect of Au-hydride formation at the interface with CeO₂.