Direct Conversion of Methane to Methanol by Metal-Exchanged ZSM-5 Zeolite (Metal = Fe, Co, Ni, Cu)

Research output: Contribution to journalArticle

43 Citations (Scopus)

Abstract

Metal-exchanged zeolites are known to exhibit catalytic activity in the direct conversion of methane to methanol. The influence of different metals on this reaction has been theoretically investigated by using density functional theory (DFT) calculations on a periodic system of MO+-ZSM-5 zeolite (M = Fe, Co, Ni, Cu). The results indicate a high dependence of the reaction on the metals, where the reactivity toward C-H bond dissociation is predicted to increase in the order CoO+-ZSM-5 < NiO+-ZSM-5 < FeO+-ZSM-5 < CuO+-ZSM-5 and the selectivity of methanol is predicted to increase in the order FeO+-ZSM-5 < CoO+-ZSM-5 < NiO+-ZSM-5 < CuO+-ZSM-5. The role of ZSM-5 zeolite in the catalytic activity is also investigated by comparing our calculation results with those reported for the reaction by bare MO+ species in the gas phase. We found that the nanopores of ZSM-5 zeolite exert a confinement effect which destabilizes the adsorption of methane and lowers the activation energy for the C-H bond dissociation. In addition to the conversion of methane, we investigated the direct conversion of ethane to ethanol by FeO+-ZSM-5 and found that this reaction proceeds with a lower C-H bond activation energy and a higher product selectivity in comparison to the conversion of methane to methanol by the same catalyst. (Chemical Equation Presented).

Original languageEnglish
Pages (from-to)8321-8331
Number of pages11
JournalACS Catalysis
Volume6
Issue number12
DOIs
Publication statusPublished - Dec 2 2016

Fingerprint

Methane
Methanol
Metals
Catalyst activity
Activation energy
Zeolites
Ethane
Nanopores
Time varying systems
Density functional theory
Ethanol
Gases
Adsorption
Catalysts
ZSM-5 zeolite

All Science Journal Classification (ASJC) codes

  • Catalysis

Cite this

Direct Conversion of Methane to Methanol by Metal-Exchanged ZSM-5 Zeolite (Metal = Fe, Co, Ni, Cu). / Mahyuddin, M. Haris; Staykov, Aleksandar Tsekov; Shiota, Yoshihito; Yoshizawa, Kazunari.

In: ACS Catalysis, Vol. 6, No. 12, 02.12.2016, p. 8321-8331.

Research output: Contribution to journalArticle

@article{46ca34b517c943ab8b20c72bca3da63a,
title = "Direct Conversion of Methane to Methanol by Metal-Exchanged ZSM-5 Zeolite (Metal = Fe, Co, Ni, Cu)",
abstract = "Metal-exchanged zeolites are known to exhibit catalytic activity in the direct conversion of methane to methanol. The influence of different metals on this reaction has been theoretically investigated by using density functional theory (DFT) calculations on a periodic system of MO+-ZSM-5 zeolite (M = Fe, Co, Ni, Cu). The results indicate a high dependence of the reaction on the metals, where the reactivity toward C-H bond dissociation is predicted to increase in the order CoO+-ZSM-5 < NiO+-ZSM-5 < FeO+-ZSM-5 < CuO+-ZSM-5 and the selectivity of methanol is predicted to increase in the order FeO+-ZSM-5 < CoO+-ZSM-5 < NiO+-ZSM-5 < CuO+-ZSM-5. The role of ZSM-5 zeolite in the catalytic activity is also investigated by comparing our calculation results with those reported for the reaction by bare MO+ species in the gas phase. We found that the nanopores of ZSM-5 zeolite exert a confinement effect which destabilizes the adsorption of methane and lowers the activation energy for the C-H bond dissociation. In addition to the conversion of methane, we investigated the direct conversion of ethane to ethanol by FeO+-ZSM-5 and found that this reaction proceeds with a lower C-H bond activation energy and a higher product selectivity in comparison to the conversion of methane to methanol by the same catalyst. (Chemical Equation Presented).",
author = "Mahyuddin, {M. Haris} and Staykov, {Aleksandar Tsekov} and Yoshihito Shiota and Kazunari Yoshizawa",
year = "2016",
month = "12",
day = "2",
doi = "10.1021/acscatal.6b01721",
language = "English",
volume = "6",
pages = "8321--8331",
journal = "ACS Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "12",

}

TY - JOUR

T1 - Direct Conversion of Methane to Methanol by Metal-Exchanged ZSM-5 Zeolite (Metal = Fe, Co, Ni, Cu)

AU - Mahyuddin, M. Haris

AU - Staykov, Aleksandar Tsekov

AU - Shiota, Yoshihito

AU - Yoshizawa, Kazunari

PY - 2016/12/2

Y1 - 2016/12/2

N2 - Metal-exchanged zeolites are known to exhibit catalytic activity in the direct conversion of methane to methanol. The influence of different metals on this reaction has been theoretically investigated by using density functional theory (DFT) calculations on a periodic system of MO+-ZSM-5 zeolite (M = Fe, Co, Ni, Cu). The results indicate a high dependence of the reaction on the metals, where the reactivity toward C-H bond dissociation is predicted to increase in the order CoO+-ZSM-5 < NiO+-ZSM-5 < FeO+-ZSM-5 < CuO+-ZSM-5 and the selectivity of methanol is predicted to increase in the order FeO+-ZSM-5 < CoO+-ZSM-5 < NiO+-ZSM-5 < CuO+-ZSM-5. The role of ZSM-5 zeolite in the catalytic activity is also investigated by comparing our calculation results with those reported for the reaction by bare MO+ species in the gas phase. We found that the nanopores of ZSM-5 zeolite exert a confinement effect which destabilizes the adsorption of methane and lowers the activation energy for the C-H bond dissociation. In addition to the conversion of methane, we investigated the direct conversion of ethane to ethanol by FeO+-ZSM-5 and found that this reaction proceeds with a lower C-H bond activation energy and a higher product selectivity in comparison to the conversion of methane to methanol by the same catalyst. (Chemical Equation Presented).

AB - Metal-exchanged zeolites are known to exhibit catalytic activity in the direct conversion of methane to methanol. The influence of different metals on this reaction has been theoretically investigated by using density functional theory (DFT) calculations on a periodic system of MO+-ZSM-5 zeolite (M = Fe, Co, Ni, Cu). The results indicate a high dependence of the reaction on the metals, where the reactivity toward C-H bond dissociation is predicted to increase in the order CoO+-ZSM-5 < NiO+-ZSM-5 < FeO+-ZSM-5 < CuO+-ZSM-5 and the selectivity of methanol is predicted to increase in the order FeO+-ZSM-5 < CoO+-ZSM-5 < NiO+-ZSM-5 < CuO+-ZSM-5. The role of ZSM-5 zeolite in the catalytic activity is also investigated by comparing our calculation results with those reported for the reaction by bare MO+ species in the gas phase. We found that the nanopores of ZSM-5 zeolite exert a confinement effect which destabilizes the adsorption of methane and lowers the activation energy for the C-H bond dissociation. In addition to the conversion of methane, we investigated the direct conversion of ethane to ethanol by FeO+-ZSM-5 and found that this reaction proceeds with a lower C-H bond activation energy and a higher product selectivity in comparison to the conversion of methane to methanol by the same catalyst. (Chemical Equation Presented).

UR - http://www.scopus.com/inward/record.url?scp=85002388996&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85002388996&partnerID=8YFLogxK

U2 - 10.1021/acscatal.6b01721

DO - 10.1021/acscatal.6b01721

M3 - Article

VL - 6

SP - 8321

EP - 8331

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 12

ER -