0562674 - ÚFCH JH 2024 RIV GB eng J - Článek v odborném periodiku
Jašík, Juraj - Valtera, Stanislav - Vaidulych, Mykhailo - Bunian, M. - Lei, Y. - Halder, A. - Tarábková, Hana - Jindra, Martin - Kavan, Ladislav - Frank, Otakar - Bartling, S. - Vajda, Štefan
Oxidative dehydrogenation of cyclohexene on atomically precise subnanometer Cu4-nPdn (0 <= n <= 4) tetramer clusters: the effect of cluster composition and support on performance.
Faraday Discussions. Roč. 242, JAN 2023 (2023), s. 70-93. ISSN 1359-6640. E-ISSN 1364-5498
Grant CEP: GA MŠMT EF16_026/0008382
GRANT EU: European Commission(XE) 810310 - J. Heyrovsky Chair
Grant ostatní: Ministerstvo školství, mládeže a tělovýchovy - GA MŠk(CZ) CZ.02.1.01/0.0/0.0/16_026/0008382
Institucionální podpora: RVO:61388955
Klíčová slova: PALLADIUM CLUSTERS * PARTICLE-SIZE * STRUCTURE SENSITIVITY
Obor OECD: Physical chemistry
Impakt faktor: 3.3, rok: 2023 ; AIS: 0.87, rok: 2023
Způsob publikování: Open access
DOI: https://doi.org/10.1039/d2fd00108j

The pronounced effects of the composition of four-atom monometallic Cu and Pd and bimetallic CuPd clusters and the support on the catalytic activity and selectivity in the oxidative dehydrogenation of cyclohexene are reported. The ultra-nanocrystalline diamond supported clusters are highly active and dominantly produce benzene, some of the mixed clusters also produce cyclohexadiene, which are all clusters with a much suppressed combustion channel. The also highly active TiO2-supported tetramers solely produce benzene, without any combustion to CO2. The selectivity of the zirconia-supported mixed CuPd clusters and the monometallic Cu cluster is entirely different, though they are less active in comparison to clusters with other supports, these clusters produce significant fractions of cyclohexadiene, with their selectivity towards cyclohexadiene gradually increasing with the increasing number of copper atoms in the cluster, reaching about 50% for Cu3Pd1. The zirconia-supported copper tetramer stands out from among all the other tetramers in this reaction, with a selectivity towards cyclohexadiene of 70%, which far exceeds those of all the other cluster-support combinations. The findings from this study indicate a positive effect of copper on the stability of the mixed tetramers and potential new ways of fine-tuning catalyst performance by controlling the composition of the active site and via cluster-support interactions in complex oxidative reactions under the suppression of the undesired combustion of the feed.
Trvalý link: https://hdl.handle.net/11104/0334928