Catalytic Dehydration of 2-Propanol by Size-Selected (WO3)n and (MoO3)n Metal Oxide Clusters

Tang, Xin; Bumueller, Dennis; Lim, Alane; Schneider, John; Heiz, Ulrich; Ganteför, Gerd; Fairbrother, D. Howard; Bowen, Kit H.

Catalytic Dehydration of 2-Propanol by Size-Selected (WO₃)_n and (MoO₃)_n Metal Oxide Clusters

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Datum

2014

Autor:innen

Tang, Xin

Bumueller, Dennis

Lim, Alane

Schneider, John

Heiz, Ulrich

Ganteför, Gerd

Fairbrother, D. Howard

Bowen, Kit H.

DOI (zitierfähiger Link)

https://doi.org/10.1021/jp505440g

Sammlungen

Physik

Publikationstyp

Zeitschriftenartikel

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Journal of Chemical Physics C. 2014, 118(50), pp. 29278-29286. ISSN 0021-9606. eISSN 1089-7690. Available under: doi: 10.1021/jp505440g

Zusammenfassung

Here, we report the catalytic dehydration of 2-propanol by metal oxide clusters, (WO₃)_n and (MoO₃)_n (n = 1, 2, 3, 5, 30), prepared by mass selecting and soft-landing metal oxide cluster anions created in the gas phase. Temperature-programmed reaction (TPR) was used to characterize the catalytic activity of the deposited clusters by measuring the production of propene from 2-propanol. The nature of the support, thermal history, size of the cluster, and cluster composition were all found to play important roles in influencing catalytic activity. (WO₃)₃ clusters deposited on HOPG (highly ordered pyrolytic graphite) and oxide supports exhibited catalytic activity, although (WO₃)₁ monomers deposited on HOPG did not catalyze 2-propanol dehydration effectively, an effect ascribed to their coalescence into large aggregates on HOPG. For tungsten oxide clusters deposited on annealed oxide films, catalytic activity was observed for all cluster sizes and was linearly correlated with the size of the deposited clusters. Two different mechanisms, linear-scaling of active sites and cluster ripening, could account for this linear dependence. However, even on oxide supports, deposited tungsten oxide clusters lost catalytic activity after annealing to 400 °C. The effect is consistent with the loss of dioxo groups rather than any cluster aggregation. Compared to tungsten oxide clusters, molybdenum oxide clusters exhibited little or no catalytic activity toward the dehydration of 2-propanol, rationalized by the decrease in Lewis acidity of molybdenum–oxygen bonds.

Fachgebiet (DDC)

530 Physik

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ISO 690

TANG, Xin, Dennis BUMUELLER, Alane LIM, John SCHNEIDER, Ulrich HEIZ, Gerd GANTEFÖR, D. Howard FAIRBROTHER, Kit H. BOWEN, 2014. Catalytic Dehydration of 2-Propanol by Size-Selected (WO₃)_n and (MoO₃)_n Metal Oxide Clusters. In: Journal of Chemical Physics C. 2014, 118(50), pp. 29278-29286. ISSN 0021-9606. eISSN 1089-7690. Available under: doi: 10.1021/jp505440g

BibTex

@article{Tang2014Catal-31293,
  year={2014},
  doi={10.1021/jp505440g},
  title={Catalytic Dehydration of 2-Propanol by Size-Selected (WO<sub>3</sub>)<sub>n</sub> and (MoO<sub>3</sub>)<sub>n</sub> Metal Oxide Clusters},
  number={50},
  volume={118},
  issn={0021-9606},
  journal={Journal of Chemical Physics C},
  pages={29278--29286},
  author={Tang, Xin and Bumueller, Dennis and Lim, Alane and Schneider, John and Heiz, Ulrich and Ganteför, Gerd and Fairbrother, D. Howard and Bowen, Kit H.}
}

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