Reaction mechanism between small-sized Ce clusters and water molecules: An: ab initio investigation on Ce n +H 2 O

Rulong Zhou, Yang Yang, Seema Pande, Bingyan Qu, Dongdong Li, Xiao Cheng Zeng

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Reactions of small-sized cerium clusters Ce n (n = 1-3) with a single water molecule are systematically investigated theoretically. The ground state structures of the Ce n /H 2 O complex and the reaction pathways between Ce n + H 2 O are predicted. Our results show the size-dependent reactivity of small-sized Ce clusters. The calculated reaction energies and reaction barriers indicate that the reactivity between Ce n and water becomes higher with increasing cluster size. The predicted reaction pathways show that the single Ce atom and the Ce 2 and Ce 3 clusters can all easily react with H 2 O and dissociate the water molecule. Under UV-irradiation, the reaction of a Ce atom with a single H 2 O molecule may even release an H 2 molecule. The reaction of either Ce 2 or Ce 3 with a single H 2 O molecule can fully dissociate the H 2 O into H and O atoms while it is bonded with the Ce cluster. The electronic configuration and oxidation states of the Ce atoms in the products and the higher occupied molecular orbitals are analyzed by using the natural bond orbital (NBO) analysis method, from which the high reactivity between the reaction products of Ce n + H 2 O and an additional H 2 O molecule is predicted. Our results offer deeper molecular insights into the chemical reactivity of Ce, which could be helpful for developing more efficient Ce-doped or Ce-based catalysts.

Original languageEnglish (US)
Pages (from-to)4006-4014
Number of pages9
JournalPhysical Chemistry Chemical Physics
Volume21
Issue number7
DOIs
StatePublished - Jan 1 2019

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Molecules
Water
water
reactivity
molecules
Atoms
atoms
Cerium
Chemical reactivity
Molecular orbitals
Reaction products
Ground state
cerium
reaction products
Irradiation
molecular orbitals
Oxidation
Catalysts
catalysts
orbitals

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Reaction mechanism between small-sized Ce clusters and water molecules : An: ab initio investigation on Ce n +H 2 O. / Zhou, Rulong; Yang, Yang; Pande, Seema; Qu, Bingyan; Li, Dongdong; Zeng, Xiao Cheng.

In: Physical Chemistry Chemical Physics, Vol. 21, No. 7, 01.01.2019, p. 4006-4014.

Research output: Contribution to journalArticle

Zhou, Rulong ; Yang, Yang ; Pande, Seema ; Qu, Bingyan ; Li, Dongdong ; Zeng, Xiao Cheng. / Reaction mechanism between small-sized Ce clusters and water molecules : An: ab initio investigation on Ce n +H 2 O. In: Physical Chemistry Chemical Physics. 2019 ; Vol. 21, No. 7. pp. 4006-4014.
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