Size-Dependent Oxidative Stability of Silicon Nanoclusters Mixed with a Tantalum Atom

Masahiro Shibuta, Maximilian Huber, Toshiaki Kamoshida, Kazuya Terasaka, Miho Hatanaka, Gereon Niedner-Schatteburg, Atsushi Nakajima

Research output: Contribution to journalArticlepeer-review

Abstract

Metal-encapsulating silicon cage (M@Si16) nanoclusters (NCs) are promising superatoms (SAs) as function-tunable nanomaterials, which exhibit a superior chemical stability owing to electronic and geometric closures. Here, we examine how the superatomic nature of an alkali-like Ta@Si16SA is staggered by the variation of the number of Si atoms in TaSinNCs (n = 6, 8, 12, 15, 17, and 18) and subsequent immobilization on a C60fullerene substrate. Using X-ray photoelectron spectroscopy, the size dependence of chemical robustness of TaSinNCs on C60against O2exposures is quantitatively evaluated: In addition to the most outstanding stability of a Ta@Si16SA as compared to TaSi15, some enhanced stability is also observed at Ta@Si17, which couples in a Si-adatom structure of (Ta@Si16)-Si to the support. While oxidative reactivities of TaSinare gradually suppressed from small NCs (n = 6) to larger ones (n = 18) with increasing number of Si atoms, the results show that (1) an enclosing Si cage around a Ta atom is completed at Ta@Si16on C60and (2) Ta@Si17NCs are robust against O2oxidation with assistance from the stability of Ta@Si16SA despite the Si-adatom.

Original languageEnglish
Pages (from-to)4423-4432
Number of pages10
JournalJournal of Physical Chemistry C
Volume126
Issue number9
DOIs
Publication statusPublished - 2022 Mar 10
Externally publishedYes

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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