Temperature-programmed oxidation of coked noble metal catalysts after autothermal reforming of n-hexadecane

E. I. Kauppi, Reetta Kaila, J. A. Linnekoski, A. O. I. Krause, M. K. Veringa Niemelä

Research output: Contribution to journalArticleScientificpeer-review

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Abstract

Autothermal reforming (ATR) of n-hexadecane was carried out on zirconia-supported mono- and bimetallic noble metal (Rh, Pt) catalysts at 600, 700, and 800 °C. After ATR, the reactivity of coke deposits (2.8–9.9 wt%) on the catalysts was investigated by temperature-programmed oxidation (TPO). Analysis of the results obtained from ATR and TPO experiments at various temperatures and on the different catalysts gave information on the reaction conditions where the detrimental coke can be minimized and allows estimating the nature of carbon deposits.

H2 production increased with temperature on the tested Rh-containing catalysts and the ZrO2 support, but decreased as a function of temperature on the Pt catalyst. The formation of coke was least at 800 °C, evidently due to the intensifying reaction of carbon and steam with increasing temperature, as well as to the better activity of the catalysts. The amount of coke formed was highest at 700 °C. Comparison of the TPO profiles obtained for the monometallic Rh and Pt catalysts with the bimetallic RhPt revealed differences in the nature of carbon deposits on their surface. At 600 °C, the coke formed on the monometallic Rh and Pt catalysts was located mostly on the support, whereas on the bimetallic RhPt catalyst the formation of this type of coke was suppressed. The bimetallic RhPt catalyst also exhibited better tolerance toward coking at 700 °C. Therefore, although the selectivity toward hydrogen was not related to the amount of coke formed, the deactivation patterns differed on the mono- and bimetallic catalysts.

Original languageEnglish
Pages (from-to)7759-7767
JournalInternational Journal of Hydrogen Energy
Volume35
Issue number15
DOIs
Publication statusPublished - 2010
MoE publication typeA1 Journal article-refereed
Event10th Chinese Hydrogen Energy Conference, CHEC - Tianjin, China
Duration: 17 Sep 200920 Sep 2009

Fingerprint

Reforming reactions
Precious metals
noble metals
coke
catalysts
Oxidation
Coke
oxidation
Catalysts
Temperature
temperature
Deposits
deposits
Catalyst supports
Carbon
carbon
Coking
zirconium oxides
steam
Zirconia

Keywords

  • ATR
  • Mono- and bimetallic
  • Pt
  • Rh
  • TPO
  • Zirconia

Cite this

Kauppi, E. I. ; Kaila, Reetta ; Linnekoski, J. A. ; Krause, A. O. I. ; Veringa Niemelä, M. K. / Temperature-programmed oxidation of coked noble metal catalysts after autothermal reforming of n-hexadecane. In: International Journal of Hydrogen Energy. 2010 ; Vol. 35, No. 15. pp. 7759-7767.
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title = "Temperature-programmed oxidation of coked noble metal catalysts after autothermal reforming of n-hexadecane",
abstract = "Autothermal reforming (ATR) of n-hexadecane was carried out on zirconia-supported mono- and bimetallic noble metal (Rh, Pt) catalysts at 600, 700, and 800 °C. After ATR, the reactivity of coke deposits (2.8–9.9 wt{\%}) on the catalysts was investigated by temperature-programmed oxidation (TPO). Analysis of the results obtained from ATR and TPO experiments at various temperatures and on the different catalysts gave information on the reaction conditions where the detrimental coke can be minimized and allows estimating the nature of carbon deposits.H2 production increased with temperature on the tested Rh-containing catalysts and the ZrO2 support, but decreased as a function of temperature on the Pt catalyst. The formation of coke was least at 800 °C, evidently due to the intensifying reaction of carbon and steam with increasing temperature, as well as to the better activity of the catalysts. The amount of coke formed was highest at 700 °C. Comparison of the TPO profiles obtained for the monometallic Rh and Pt catalysts with the bimetallic RhPt revealed differences in the nature of carbon deposits on their surface. At 600 °C, the coke formed on the monometallic Rh and Pt catalysts was located mostly on the support, whereas on the bimetallic RhPt catalyst the formation of this type of coke was suppressed. The bimetallic RhPt catalyst also exhibited better tolerance toward coking at 700 °C. Therefore, although the selectivity toward hydrogen was not related to the amount of coke formed, the deactivation patterns differed on the mono- and bimetallic catalysts.",
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author = "Kauppi, {E. I.} and Reetta Kaila and Linnekoski, {J. A.} and Krause, {A. O. I.} and {Veringa Niemel{\"a}}, {M. K.}",
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language = "English",
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Temperature-programmed oxidation of coked noble metal catalysts after autothermal reforming of n-hexadecane. / Kauppi, E. I.; Kaila, Reetta; Linnekoski, J. A.; Krause, A. O. I.; Veringa Niemelä, M. K.

In: International Journal of Hydrogen Energy, Vol. 35, No. 15, 2010, p. 7759-7767.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - Temperature-programmed oxidation of coked noble metal catalysts after autothermal reforming of n-hexadecane

AU - Kauppi, E. I.

AU - Kaila, Reetta

AU - Linnekoski, J. A.

AU - Krause, A. O. I.

AU - Veringa Niemelä, M. K.

PY - 2010

Y1 - 2010

N2 - Autothermal reforming (ATR) of n-hexadecane was carried out on zirconia-supported mono- and bimetallic noble metal (Rh, Pt) catalysts at 600, 700, and 800 °C. After ATR, the reactivity of coke deposits (2.8–9.9 wt%) on the catalysts was investigated by temperature-programmed oxidation (TPO). Analysis of the results obtained from ATR and TPO experiments at various temperatures and on the different catalysts gave information on the reaction conditions where the detrimental coke can be minimized and allows estimating the nature of carbon deposits.H2 production increased with temperature on the tested Rh-containing catalysts and the ZrO2 support, but decreased as a function of temperature on the Pt catalyst. The formation of coke was least at 800 °C, evidently due to the intensifying reaction of carbon and steam with increasing temperature, as well as to the better activity of the catalysts. The amount of coke formed was highest at 700 °C. Comparison of the TPO profiles obtained for the monometallic Rh and Pt catalysts with the bimetallic RhPt revealed differences in the nature of carbon deposits on their surface. At 600 °C, the coke formed on the monometallic Rh and Pt catalysts was located mostly on the support, whereas on the bimetallic RhPt catalyst the formation of this type of coke was suppressed. The bimetallic RhPt catalyst also exhibited better tolerance toward coking at 700 °C. Therefore, although the selectivity toward hydrogen was not related to the amount of coke formed, the deactivation patterns differed on the mono- and bimetallic catalysts.

AB - Autothermal reforming (ATR) of n-hexadecane was carried out on zirconia-supported mono- and bimetallic noble metal (Rh, Pt) catalysts at 600, 700, and 800 °C. After ATR, the reactivity of coke deposits (2.8–9.9 wt%) on the catalysts was investigated by temperature-programmed oxidation (TPO). Analysis of the results obtained from ATR and TPO experiments at various temperatures and on the different catalysts gave information on the reaction conditions where the detrimental coke can be minimized and allows estimating the nature of carbon deposits.H2 production increased with temperature on the tested Rh-containing catalysts and the ZrO2 support, but decreased as a function of temperature on the Pt catalyst. The formation of coke was least at 800 °C, evidently due to the intensifying reaction of carbon and steam with increasing temperature, as well as to the better activity of the catalysts. The amount of coke formed was highest at 700 °C. Comparison of the TPO profiles obtained for the monometallic Rh and Pt catalysts with the bimetallic RhPt revealed differences in the nature of carbon deposits on their surface. At 600 °C, the coke formed on the monometallic Rh and Pt catalysts was located mostly on the support, whereas on the bimetallic RhPt catalyst the formation of this type of coke was suppressed. The bimetallic RhPt catalyst also exhibited better tolerance toward coking at 700 °C. Therefore, although the selectivity toward hydrogen was not related to the amount of coke formed, the deactivation patterns differed on the mono- and bimetallic catalysts.

KW - ATR

KW - Mono- and bimetallic

KW - Pt

KW - Rh

KW - TPO

KW - Zirconia

U2 - 10.1016/j.ijhydene.2010.05.046

DO - 10.1016/j.ijhydene.2010.05.046

M3 - Article

VL - 35

SP - 7759

EP - 7767

JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

SN - 0360-3199

IS - 15

ER -