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Oxidative Dehydrogenation of Cyclohexane by Cu vs Pd Clusters: Selectivity Control by Specific Cluster Dynamics
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SYSNO ASEP 0523057 Druh ASEP J - Článek v odborném periodiku Zařazení RIV J - Článek v odborném periodiku Poddruh J Článek ve WOS Název Oxidative Dehydrogenation of Cyclohexane by Cu vs Pd Clusters: Selectivity Control by Specific Cluster Dynamics Tvůrce(i) Halder, A. (US)
Ha, M.-A. (US)
Zhai, H. (US)
Yang, B. (US)
Pellin, M. J. (US)
Seifert, S. (US)
Alexandrova, A. N. (US)
Vajda, Štefan (UFCH-W) RID, ORCIDZdroj.dok. ChemCatChem. - : Wiley - ISSN 1867-3880
Roč. 12, JAN 2020 (2020), s. 1307-1315Poč.str. 9 s. Jazyk dok. eng - angličtina Země vyd. DE - Německo Klíč. slova size ; catalysts ; reactivity ; ensemble ; ethylene ; route ; tio2 ; cluster dynamics ; cyclohexane oxidative dehydrogenation ; deposited clusters ; selectivity control ; size-selected subnanometer clusters Vědní obor RIV CF - Fyzikální chemie a teoretická chemie Obor OECD Physical chemistry Způsob publikování Open access Institucionální podpora UFCH-W - RVO:61388955 UT WOS 000505076200001 EID SCOPUS 85078066446 DOI 10.1002/cctc.201901795 Anotace Supported subnanometer clusters can exhibit catalytic properties not observed in their bulk analogues. Partially-oxidized Pd and Cu clusters are reported to catalyze the oxidative dehydrogenation of cyclohexane with high activity, and with distinctly different selectivity, producing primarily benzene or cyclohexene, respectively. Under the appliedreaction conditions, the structure and oxidation state of the two catalysts evolve differently, which leads to either the desorption of the cyclohexene intermediate or to its deeper dehydrogenation. Under the applied reaction conditions, the initially oxidized Pd and Cu clusters undergo partial reduction, which we show to be required for the selectivity to emerge. Both systems also have thermal access to multiple distinct structural forms yielding statistical ensembles. The structures within these ensembles evolve with the changing nature of the bound reaction intermediates differently for the two metals. The evolution is found pronounced in the Cu clusters, but only modest in Pd. Ultimately, the different selectivity observed experimentally for the Cu versus Pd clusters is controlled by differences in the collective structural and redox dynamics of their ensembles. Pracoviště Ústav fyzikální chemie J.Heyrovského Kontakt Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Rok sběru 2021 Elektronická adresa http://hdl.handle.net/11104/0307465
Počet záznamů: 1