Tuning the Dissociative Action of Cationic Rh Clusters Toward NO by Substituting a Single Ta Atom

Masato Yamaguchi, Satoshi Kudoh, Ken Miyajima, Olga V. Lushchikova, Joost M. Bakker, Fumitaka Mafuné

Research output: Contribution to journalArticlepeer-review

18 Citations (Scopus)

Abstract

Modification of Rh chemical activity for decomposition of NO by alloying with Ta was studied by vibrational spectroscopy of gas-phase clusters, where one single Rh atom was substituted by Ta, with NO adsorbed. While NO adsorbs molecularly on pure Rh clusters, it was found to adsorb dissociatively on Rh n Ta + (n = 2-8) with the O bound to the Ta on-top site. A reaction path for NO decomposition obtained by density functional theory calculations for octahedral Rh 5 Ta + and Rh 6 + suggests that the Ta oxygen affinity strongly reduces the energy barrier right before bond cleavage, facilitating NO dissociation. The trend is consistent with the Bell-Evans-Polanyi principle. The addition of other less oxophilic dopant atoms could plausibly enhance catalytic reactivity of Rh.

Original languageEnglish
Pages (from-to)3476-3481
Number of pages6
JournalJournal of Physical Chemistry C
Volume123
Issue number6
DOIs
Publication statusPublished - Feb 14 2019
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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