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000873927 1001_ $$0P:(DE-Juel1)165376$$aDuchoň, Tomáš$$b0$$eCorresponding author
000873927 245__ $$aEstablishing structure-sensitivity of ceria reducibility: real-time observations of surface-hydrogen interactions
000873927 260__ $$aLondon [u.a.]$$bRSC$$c2020
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000873927 520__ $$aThe first layer of atoms on an oxide catalyst provides the first sites for adsorption of reactants and the last sites before products or oxygen are desorbed. We employ a unique combination of morphological, structural, and chemical analyses of a model ceria catalyst with different surface terminations under an H2 environment to unequivocally establish the effect of the last layer of atoms on surface reduction. (111) and (100) terminated epitaxial islands of ceria are simultaneously studied in situ allowing for a direct investigation of the structure–reducibility relationship under identical conditions. Kinetic rate constants of Ce4+ to Ce3+ transformation and equilibrium concentrations are extracted for both surface terminations. Unlike the kinetic rate constants, which are practically the same for both types of islands, more pronounced oxygen release, and overall higher reducibility were observed for (100) islands compared to (111) ones. The findings are in agreement with coordination-limited oxygen vacancy formation energies calculated by density functional theory. The results point out the important aspect of surface terminations in redox processes, with particular impact on the catalytic reactions of a variety of catalysts.
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000873927 7001_ $$0P:(DE-Juel1)164109$$aHackl, Johanna$$b1
000873927 7001_ $$0P:(DE-Juel1)166093$$aMueller, David N.$$b2
000873927 7001_ $$00000-0003-3570-0050$$aKullgren, Jolla$$b3
000873927 7001_ $$0P:(DE-HGF)0$$aDu, Dou$$b4
000873927 7001_ $$00000-0003-3991-4232$$aSenanayake, Sanjaya D.$$b5
000873927 7001_ $$0P:(DE-HGF)0$$aMouls, Caroline$$b6
000873927 7001_ $$0P:(DE-Juel1)143828$$aGottlob, Daniel M.$$b7
000873927 7001_ $$0P:(DE-Juel1)164112$$aKhan, Muhammad I.$$b8
000873927 7001_ $$0P:(DE-Juel1)130601$$aCramm, Stefan$$b9
000873927 7001_ $$0P:(DE-HGF)0$$aVeltruská, Kateřina$$b10
000873927 7001_ $$0P:(DE-HGF)0$$aMatolín, Vladimír$$b11
000873927 7001_ $$0P:(DE-Juel1)164137$$aNemšák, Slavomír$$b12
000873927 7001_ $$0P:(DE-Juel1)130948$$aSchneider, Claus M.$$b13
000873927 773__ $$0PERI:(DE-600)2702232-8$$a10.1039/C9TA11784A$$gp. 10.1039.C9TA11784A$$n11$$p5501-5507$$tJournal of materials chemistry / A Materials for energy and sustainability A$$v8$$x2050-7496$$y2020
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