Unravelling the Role of Structural Geometry and Chemical State of Well-Defined Oxygen Vacancies on Pristine CeO2 for H2O2 Activation

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Detail(s)

Original languageEnglish
Pages (from-to)5390-5396
Journal / PublicationJournal of Physical Chemistry Letters
Volume11
Issue number14
Online published17 Jun 2020
Publication statusPublished - 16 Jul 2020

Abstract

Although H2O2 has been often employed as a green oxidant for many CeO2-catalyzed reactions, the underlying principle of its activation by surface oxygen vacancy (Vo) is still elusive due to the irreversible removal of postgenerated Vo by water (or H2O2). The metastable Vo (ms-Vo) naturally preserved on pristine CeO2 surfaces was adopted herein for an in-depth study of their interplay with H2O2. Their well-defined local structures and chemical states were found facet-dependent affecting both the adsorption and subsequent activation of H2O2. It is concluded that a strong adsorption of H2O2 on ms-Vo may not guarantee its subsequent activation. The ms-Vo can be only free for the next catalytic cycle when the electron density of surface Ce is high enough to reduce/break the O-O bond of adsorbed H2O2. This explains the 211.8 and 35.8 times enhancement in H2O2 reactivity when the CeO2 surface is changed from (111) and (110) to (100).

Citation Format(s)

Unravelling the Role of Structural Geometry and Chemical State of Well-Defined Oxygen Vacancies on Pristine CeO2 for H2O2 Activation. / Tan, Zicong; Zhang, Jieru; Chen, Yu-Cheng et al.
In: Journal of Physical Chemistry Letters, Vol. 11, No. 14, 16.07.2020, p. 5390-5396.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review