Abstract

The ability to observe chemical reactions at the molecular level convincingly demonstrates the physical and chemical phenomena occurring throughout a reaction mechanism. Videos obtained through in situ transmission electron microscopy (TEM) revealed the oxidation of catalytic soot under practical reaction conditions. Carbon oxidation reactions using Ag/SiO2 or Cs2CO3/nepheline catalysts were performed at 330 °C under an O2 flow of 0.5 Pa in the TEM measurement chamber. Ag/SiO2 catalyzed the reaction at the interface of the mobile Ag species and carbon, while the Cs species was fixed on the nepheline surface during the reaction. In the latter case, carbon particles moved, remained attached to the Cs2CO3/nepheline surface, and were consumed at the interface by the oxidation reaction. Using this technique, we were able to visualize such mobile and immobile catalysis according to different mechanisms.

Highlights

  • The ability to observe chemical reactions at the molecular level convincingly demonstrates the physical and chemical phenomena occurring throughout a reaction mechanism

  • Several experiments using in situ transmission electron microscopy (TEM) have been reported: observation of catalytic reactions with gas and solid catalysts[21], crystal growth processes[22,23], and investigations of supported metal behavior[24,25]

  • We report in situ observation of catalytic particulate matter (PM) oxidation using TEM and demonstrate how PM oxidation proceeds, as well as catalysts’ behavior during oxidation

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Summary

Introduction

The ability to observe chemical reactions at the molecular level convincingly demonstrates the physical and chemical phenomena occurring throughout a reaction mechanism. Catalytic PM oxidation occurs under solid (PM, carbon)–solid (catalyst)–gas (O2) triphasic conditions when using mobile species. Real-time investigation of the reaction mechanism on solid catalysts under operating conditions and in the presence of reactants at high temperatures remains a challenge; recent studies have used in situ and operando analyses

Results
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