Abstract
To elucidate the reaction mechanism of catalytic steam reforming of methane in an electric field, operando-diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) has been used to investigate methane dissociative adsorption at low temperatures using CH4, H2O, and their isotopes. Operando-analyses demonstrated that methane was adsorbed and converted into CO and CO2 more when CD4 and/or D2O was used instead of CH4 and/or H2O. This observed "inverse" kinetic isotope effect is based on the difference of CHH vibrational energy level at the transition state. Furthermore, CO2-methanation, which is the reverse reaction of steam reforming of methane, was irreversible with H2O in an electric field. These results demonstrate that the proton collision promoted methane activation irreversibly, even at low temperatures in an electric field.
| Original language | English |
|---|---|
| Journal | Catalysis Today |
| DOIs | |
| Publication status | Accepted/In press - 2016 Sep 28 |
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Keywords
- Electric field
- Hydrogen production
- Inverse kinetic isotope effect
- Methanation
- Operando-DRIFTS
ASJC Scopus subject areas
- Catalysis
- Chemistry(all)
Cite this
Methane dissociative adsorption in catalytic steam reforming of methane over Pd/CeO2 in an electric field. / Okada, S.; Manabe, R.; Inagaki, R.; Ogo, Shuhei; Sekine, Yasushi.
In: Catalysis Today, 28.09.2016.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Methane dissociative adsorption in catalytic steam reforming of methane over Pd/CeO2 in an electric field
AU - Okada, S.
AU - Manabe, R.
AU - Inagaki, R.
AU - Ogo, Shuhei
AU - Sekine, Yasushi
PY - 2016/9/28
Y1 - 2016/9/28
N2 - To elucidate the reaction mechanism of catalytic steam reforming of methane in an electric field, operando-diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) has been used to investigate methane dissociative adsorption at low temperatures using CH4, H2O, and their isotopes. Operando-analyses demonstrated that methane was adsorbed and converted into CO and CO2 more when CD4 and/or D2O was used instead of CH4 and/or H2O. This observed "inverse" kinetic isotope effect is based on the difference of CHH vibrational energy level at the transition state. Furthermore, CO2-methanation, which is the reverse reaction of steam reforming of methane, was irreversible with H2O in an electric field. These results demonstrate that the proton collision promoted methane activation irreversibly, even at low temperatures in an electric field.
AB - To elucidate the reaction mechanism of catalytic steam reforming of methane in an electric field, operando-diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) has been used to investigate methane dissociative adsorption at low temperatures using CH4, H2O, and their isotopes. Operando-analyses demonstrated that methane was adsorbed and converted into CO and CO2 more when CD4 and/or D2O was used instead of CH4 and/or H2O. This observed "inverse" kinetic isotope effect is based on the difference of CHH vibrational energy level at the transition state. Furthermore, CO2-methanation, which is the reverse reaction of steam reforming of methane, was irreversible with H2O in an electric field. These results demonstrate that the proton collision promoted methane activation irreversibly, even at low temperatures in an electric field.
KW - Electric field
KW - Hydrogen production
KW - Inverse kinetic isotope effect
KW - Methanation
KW - Operando-DRIFTS
UR - http://www.scopus.com/inward/record.url?scp=85020452507&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85020452507&partnerID=8YFLogxK
U2 - 10.1016/j.cattod.2017.05.079
DO - 10.1016/j.cattod.2017.05.079
M3 - Article
AN - SCOPUS:85020452507
JO - Catalysis Today
JF - Catalysis Today
SN - 0920-5861
ER -