Oxidative dehydrogenation of ethane over Cr/ZSM-5 catalysts using CO2 as an oxidant

Naoki Mimura, Masaki Okamoto, Hiromi Yamashita, S. Ted Oyama, Kazuhisa Murata

Research output: Contribution to journalArticle

36 Citations (Scopus)

Abstract

Highly active catalysts for oxidative dehydrogenation of ethane with CO2 were characterized by temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), Fourier transform infrared (FTIR) spectroscopy, and X-ray absorption fine-structure (XAFS) analysis. In the active catalysts, Cr/H-ZSM-5 (SiO2/ Al2O3 > 190), Cr6+ = O, or possibly Cr5+ = O was the catalytic species on the zeolite support. In contrast, little Cr6+ (or Cr5+) was detected in the less-active catalysts. The Cr6+ (or Cr5+) species was reduced to an octahedral Cr3+ species by treatment with ethane at 773 K, and the reduced Cr species was reoxidized to the Cr6+ (or Cr5+) species by treatment with CO2 at 673-773 K. The Cr redox cycle played an important role in the catalyst's high activity.

Original languageEnglish
Pages (from-to)21764-21770
Number of pages7
JournalJournal of Physical Chemistry B
Volume110
Issue number43
DOIs
Publication statusPublished - 2006 Nov 2
Externally publishedYes

Fingerprint

Ethane
Dehydrogenation
dehydrogenation
Oxidants
ethane
Zeolites
catalysts
Catalysts
Temperature
Fourier Transform Infrared Spectroscopy
Oxidation-Reduction
X-Rays
X ray absorption
Fourier transform infrared spectroscopy
fine structure
infrared spectroscopy
Oxidation
oxidation
cycles
temperature

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

Oxidative dehydrogenation of ethane over Cr/ZSM-5 catalysts using CO2 as an oxidant. / Mimura, Naoki; Okamoto, Masaki; Yamashita, Hiromi; Ted Oyama, S.; Murata, Kazuhisa.

In: Journal of Physical Chemistry B, Vol. 110, No. 43, 02.11.2006, p. 21764-21770.

Research output: Contribution to journalArticle

Mimura, Naoki ; Okamoto, Masaki ; Yamashita, Hiromi ; Ted Oyama, S. ; Murata, Kazuhisa. / Oxidative dehydrogenation of ethane over Cr/ZSM-5 catalysts using CO2 as an oxidant. In: Journal of Physical Chemistry B. 2006 ; Vol. 110, No. 43. pp. 21764-21770.
@article{bb71c4d1918b4d3a9073e350b2b4e2b7,
title = "Oxidative dehydrogenation of ethane over Cr/ZSM-5 catalysts using CO2 as an oxidant",
abstract = "Highly active catalysts for oxidative dehydrogenation of ethane with CO2 were characterized by temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), Fourier transform infrared (FTIR) spectroscopy, and X-ray absorption fine-structure (XAFS) analysis. In the active catalysts, Cr/H-ZSM-5 (SiO2/ Al2O3 > 190), Cr6+ = O, or possibly Cr5+ = O was the catalytic species on the zeolite support. In contrast, little Cr6+ (or Cr5+) was detected in the less-active catalysts. The Cr6+ (or Cr5+) species was reduced to an octahedral Cr3+ species by treatment with ethane at 773 K, and the reduced Cr species was reoxidized to the Cr6+ (or Cr5+) species by treatment with CO2 at 673-773 K. The Cr redox cycle played an important role in the catalyst's high activity.",
author = "Naoki Mimura and Masaki Okamoto and Hiromi Yamashita and {Ted Oyama}, S. and Kazuhisa Murata",
year = "2006",
month = "11",
day = "2",
doi = "10.1021/jp061966l",
language = "English",
volume = "110",
pages = "21764--21770",
journal = "Journal of Physical Chemistry B Materials",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "43",

}

TY - JOUR

T1 - Oxidative dehydrogenation of ethane over Cr/ZSM-5 catalysts using CO2 as an oxidant

AU - Mimura, Naoki

AU - Okamoto, Masaki

AU - Yamashita, Hiromi

AU - Ted Oyama, S.

AU - Murata, Kazuhisa

PY - 2006/11/2

Y1 - 2006/11/2

N2 - Highly active catalysts for oxidative dehydrogenation of ethane with CO2 were characterized by temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), Fourier transform infrared (FTIR) spectroscopy, and X-ray absorption fine-structure (XAFS) analysis. In the active catalysts, Cr/H-ZSM-5 (SiO2/ Al2O3 > 190), Cr6+ = O, or possibly Cr5+ = O was the catalytic species on the zeolite support. In contrast, little Cr6+ (or Cr5+) was detected in the less-active catalysts. The Cr6+ (or Cr5+) species was reduced to an octahedral Cr3+ species by treatment with ethane at 773 K, and the reduced Cr species was reoxidized to the Cr6+ (or Cr5+) species by treatment with CO2 at 673-773 K. The Cr redox cycle played an important role in the catalyst's high activity.

AB - Highly active catalysts for oxidative dehydrogenation of ethane with CO2 were characterized by temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), Fourier transform infrared (FTIR) spectroscopy, and X-ray absorption fine-structure (XAFS) analysis. In the active catalysts, Cr/H-ZSM-5 (SiO2/ Al2O3 > 190), Cr6+ = O, or possibly Cr5+ = O was the catalytic species on the zeolite support. In contrast, little Cr6+ (or Cr5+) was detected in the less-active catalysts. The Cr6+ (or Cr5+) species was reduced to an octahedral Cr3+ species by treatment with ethane at 773 K, and the reduced Cr species was reoxidized to the Cr6+ (or Cr5+) species by treatment with CO2 at 673-773 K. The Cr redox cycle played an important role in the catalyst's high activity.

UR - http://www.scopus.com/inward/record.url?scp=33751274403&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=33751274403&partnerID=8YFLogxK

U2 - 10.1021/jp061966l

DO - 10.1021/jp061966l

M3 - Article

VL - 110

SP - 21764

EP - 21770

JO - Journal of Physical Chemistry B Materials

JF - Journal of Physical Chemistry B Materials

SN - 1520-6106

IS - 43

ER -