The role of the spatial arrangement of single rhodium sites on ZSM-5 in the oxidative methane carbonylation to acetic acid

Natalia V. Kolesnichenko, Tatiana I. Batova*, Anton N. Stashenko, Tatiana K. Obukhova, Evgeny V. Khramov, Alexey A. Sadovnikov, Denis E. Zavelev

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Single atom rhodium catalysts based on microporous ZSM-5 zeolite (SiO2/Al2O3 = 30) were studied in the reaction of oxidative methane carbonylation to acetic acid. For highly dispersed rhodium distribution on the zeolite surface, nitrogen-containing polymers, namely chitosan hydrochloride, polyethyleneimine, and polyvinylpyrrolidone, were used. Using XAS spectroscopy, all rhodium was found to be as single atom metal sites in the zeolite structure, which contributes to the acetic acid formation. The catalytic properties of rhodium zeolite catalysts in the oxidative methane carbonylation to acetic acid were revealed to depend not only on the single atom rhodium distribution and the catalyst acidity, but also on the spatial rhodium atom arrangement in the zeolite, which was established by the XPS. According to DFT calculations in combination with EXAFS modeling, rhodium anchored at the zeolite channel intersections was shown to be coordinated with four zeolite oxygen atoms and one hydroxyl group oxygen atom and be the dominant catalytic species in the acetic acid formation.

Original languageEnglish
Article number112239
JournalMicroporous and Mesoporous Materials
Volume344
DOIs
StatePublished - Oct 2022
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2022 Elsevier Inc.

Keywords

  • Acetic acid
  • Methane carbonylation
  • Single atom rhodium catalysts
  • Spatial arrangement of rhodium
  • ZSM-5 zeolite

Fingerprint

Dive into the research topics of 'The role of the spatial arrangement of single rhodium sites on ZSM-5 in the oxidative methane carbonylation to acetic acid'. Together they form a unique fingerprint.

Cite this