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Nanoporous Gold-Supported Ceria for the Water–Gas Shift Reaction: UHV Inspired Design for Applied Catalysis
journal contribution
posted on 2014-12-18, 00:00 authored by Junjie Shi, Andreas Schaefer, Andre Wichmann, M. Mangir Murshed, Thorsten
M. Gesing, Arne Wittstock, Marcus BäumerInspired by model studies under ultrahigh
vacuum (UHV) conditions, inverse monolithic gold/ceria catalysts are
prepared using thermal decomposition of a cerium nitrate precursor
on a nanoporous gold (npAu) substrate. Cerium oxide deposits throughout
the porous gold material (pores and ligaments 30–40 nm) are
formed. npAu disks and coatings were prepared with loadings of about
3 to 10 atom % of ceria. The composite material was tested for the
water–gas shift (WGS) reaction (H2O + CO →
H2 + CO2) in a continuous flow reactor at ambient
pressure conditions. Formation of CO2 was observed at temperatures
as low as 135 °C with excellent stability and reproducibility
up to temperatures of 535 °C. The considerably increased thermal
stability of the material can be linked to the presence of metal oxide
deposits on the nanosized gold ligaments. The loss of activity after
about 15 h of catalytic conversion with heating to 535 °C was
only about 10%. Photoemission spectroscopy indicates a defect (Ce3+) concentration of about 70% on the surface of the cerium
oxide deposits, prior to and after WGS reaction. Raman spectroscopic
characterization of the material revealed that the bulk of the oxide
is reoxidized during reaction.
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metal oxide depositsstabilitynpAu disksRaman spectroscopic characterizationWGS reactionflow reactormodel studiesCerium oxide depositscerium oxide depositsCO 2ultrahigh vacuumUHVcerium nitrate precursorH 2O15 hgold materialambient pressure conditionsApplied CatalysisInspirednanosized gold ligamentsnanoporous gold
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