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

doi:10.1021/jp061966l

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 journal › Article › peer-review

68 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 language	English
Pages (from-to)	21764-21770
Number of pages	7
Journal	Journal of Physical Chemistry B
Volume	110
Issue number	43
DOIs	https://doi.org/10.1021/jp061966l
Publication status	Published - 2006 Nov 2
Externally published	Yes

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

Access to Document

10.1021/jp061966l

Cite this

@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 = nov,

day = "2",

doi = "10.1021/jp061966l",

language = "English",

volume = "110",

pages = "21764--21770",

journal = "Journal of Physical Chemistry B",

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

AN - SCOPUS:33751274403

SN - 1520-6106

VL - 110

SP - 21764

EP - 21770

JO - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

IS - 43

ER -

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

Abstract

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this