Dependence on Size of Supported Rh Nanoclusters in the Dehydrogenation of Methanol- d4Obstructed by CO

Guan Jr Liao, Kuan Ting Liu, Zhen He Liao, Po Wei Hsu, Jeng Han Wang, Meng Fan Luo*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

The size effect on the activity of a catalyst has been a focal issue since ideal catalysts were pursued, whereas that on the degradation of a catalyst, by reaction intermediates such as CO, is little discussed. We demonstrate that the dehydrogenation of methanol-d4 on supported Rh nanoclusters precovered with CO (Rh-CO clusters) was obstructed, indicated by a decreased production of CO and D2; the obstructive effect exhibits a remarkable dependence on the cluster size, with a minimum at a cluster diameter near 1.4 nm. The decreased production arose from a decreased reaction probability controlled by the increased activation energy for each dehydrogenation step (including formation of methoxy-d3), adsorption energies of CO, and repulsion from the CO array on the Rh-CO surface. The effects of these factors in deactivating the clusters varied separately with the cluster size. Consequently, the size effect on the CO poisoning should be taken into account in engineering the cluster size to optimize the catalytic performance.

Original languageEnglish
Pages (from-to)2622-2629
Number of pages8
JournalJournal of Physical Chemistry Letters
Volume12
Issue number10
DOIs
Publication statusPublished - 2021 Mar 18

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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