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@ARTICLE{Ducho:873927,
author = {Duchoň, Tomáš and Hackl, Johanna and Mueller, David N.
and Kullgren, Jolla and Du, Dou and Senanayake, Sanjaya D.
and Mouls, Caroline and Gottlob, Daniel M. and Khan,
Muhammad I. and Cramm, Stefan and Veltruská, Kateřina and
Matolín, Vladimír and Nemšák, Slavomír and Schneider,
Claus M.},
title = {{E}stablishing structure-sensitivity of ceria reducibility:
real-time observations of surface-hydrogen interactions},
journal = {Journal of materials chemistry / A Materials for energy and
sustainability A},
volume = {8},
number = {11},
issn = {2050-7496},
address = {London [u.a.]},
publisher = {RSC},
reportid = {FZJ-2020-01101},
pages = {5501-5507},
year = {2020},
abstract = {The first layer of atoms on an oxide catalyst provides the
first sites for adsorption of reactants and the last sites
before products or oxygen are desorbed. We employ a unique
combination of morphological, structural, and chemical
analyses of a model ceria catalyst with different surface
terminations under an H2 environment to unequivocally
establish the effect of the last layer of atoms on surface
reduction. (111) and (100) terminated epitaxial islands of
ceria are simultaneously studied in situ allowing for a
direct investigation of the structure–reducibility
relationship under identical conditions. Kinetic rate
constants of Ce4+ to Ce3+ transformation and equilibrium
concentrations are extracted for both surface terminations.
Unlike the kinetic rate constants, which are practically the
same for both types of islands, more pronounced oxygen
release, and overall higher reducibility were observed for
(100) islands compared to (111) ones. The findings are in
agreement with coordination-limited oxygen vacancy formation
energies calculated by density functional theory. The
results point out the important aspect of surface
terminations in redox processes, with particular impact on
the catalytic reactions of a variety of catalysts.},
cin = {PGI-6},
ddc = {530},
cid = {I:(DE-Juel1)PGI-6-20110106},
pnm = {522 - Controlling Spin-Based Phenomena (POF3-522)},
pid = {G:(DE-HGF)POF3-522},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000521109000036},
doi = {10.1039/C9TA11784A},
url = {https://juser.fz-juelich.de/record/873927},
}