In Situ TEM study of Rh particle sintering for three-way catalysts in high temperatures

Hiroki Nakayama, Makoto Nagata, Hideki Abe, Yukihiro Shimizu

Research output: Contribution to journalArticlepeer-review

Abstract

One of the main factors in the deterioration of automobile three-way catalysts is the sintering of platinum group metals (PGMs). In this study, we used in situ tunneling electron microscopy (TEM) to examine the sintering of Rh particles as the temperature increases. Two types of environmental conditions were tested, namely, vacuum atmosphere with heating up to 1050 °C, and N2 with/without 1% O2 at 1 atm and up to 1000 °C. Under vacuum, Rh particles appeared to be immersed in ZrO2. In contrast, at 1 atm N2 with or without 1% O2, the sintered Rh particles appeared spherical and not immersed in ZrO2. The latter trend of Rh sintering resembles the actual engine-aged catalyst observed ex situ in this study. In the N2 atmosphere, the sintering of support material (ZrO2 or Y-ZrO2) was first observed by in situ TEM, followed by Rh particle sintering. The Rh particle size was slightly smaller on Y-ZrO2 compared to that on ZrO2. To better understand these experimental results, density functional theory was used to calculate the systems’ junction energies, assuming three layers of Rh(111) 4 × 4 structures joined to the support material (ZrO2 and Y-ZrO2). The calculated energies were consistent with the in situ TEM observations in the N2 atmosphere.

Original languageEnglish
Article number19
Pages (from-to)1-16
Number of pages16
JournalCatalysts
Volume11
Issue number1
DOIs
Publication statusPublished - 2021 Jan

Keywords

  • Automotive catalyst
  • DFT calculation
  • In situ TEM
  • Rh sintering
  • SMSI (strong metalsupport interaction)

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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