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Establishing structure-sensitivity of ceria reducibility : real-time observations of surface hydrogen interactions

Duchon, Tomas (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany;Charles Univ Prague, Fac Math & Phys, Dept Surface & Plasma Sci, Prague 18000, Czech Republic
Hackl, Johanna (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany
Mueller, David N. (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany
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Kullgren, Jolla, 1978- (author)
Uppsala universitet,Strukturkemi
Du, Dou (author)
Uppsala universitet,Strukturkemi
Senanayake, Sanjaya D. (author)
Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
Mouls, Caroline (author)
Uppsala universitet,Institutionen för kemi - Ångström,Lab Nacl Luz Sincrotron, BR-13083 Campinas, SP, Brazil
Gottlob, Daniel M. (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany
Khan, Muhammad I. (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany
Cramm, Stefan (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany
Veltruska, Katerina (author)
Charles Univ Prague, Fac Math & Phys, Dept Surface & Plasma Sci, Prague 18000, Czech Republic
Matolin, Vladimir (author)
Charles Univ Prague, Fac Math & Phys, Dept Surface & Plasma Sci, Prague 18000, Czech Republic
Nemsak, Slavomir (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany;Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA
Schneider, Claus M. (author)
Forschungszentrum Julich, Peter Grunberg Inst 6, D-52425 Julich, Germany;Univ Calif Davis, Dept Phys, Davis, CA 95616 USA
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 (creator_code:org_t)
2020
2020
English.
In: Journal of Materials Chemistry A. - : ROYAL SOC CHEMISTRY. - 2050-7488 .- 2050-7496. ; 8:11, s. 5501-5507
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • 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.

Subject headings

NATURVETENSKAP  -- Kemi -- Materialkemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Materials Chemistry (hsv//eng)
NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)

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