Research output: Contribution to journal › Article › peer-review
Kinetic assessment of dry reforming of methane on Pt+Ni containing composite of fluorite-like structure. / Bobrova, L. N.; Bobin, A. S.; Mezentseva, N. V. et al.
In: Applied Catalysis B: Environmental, Vol. 182, 01.03.2016, p. 513-524.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Kinetic assessment of dry reforming of methane on Pt+Ni containing composite of fluorite-like structure
AU - Bobrova, L. N.
AU - Bobin, A. S.
AU - Mezentseva, N. V.
AU - Sadykov, V. A.
AU - Thybaut, J. W.
AU - Marin, G. B.
PY - 2016/3/1
Y1 - 2016/3/1
N2 - Methane dry reforming kinetics over the 1.2% Pt/80% Pr0.15Sm0.15Ce0.35Zr0.35Ox+10%NiO+10% YSZ catalyst (Pt+Ni/PrSmCeZrO/YSZ) has been assessed. First-order kinetics in methane was found for the forward reaction rate up to an equimolar methane/carbon dioxide feed ratio. The reaction rate was inhibited by adding methane beyond the stoichiometric value. A relatively constant zero reaction order towards CO2 can be applied when a CO2 excess of at least 1.5 over the stoichiometric value is employed. The existence of two different activation regimes is evident in Arrhenius plots with an inflection point at about 750°C. Kinetic parameters for the net rate of CH4 conversion over the Pt+Ni/PrSmCeZrO/YSZ composite catalyst were also determined by regression. The novel Pt+Ni/PrSmCeZrO/YSZ catalyst was benchmarked against a complex Pt-promoted fluorite-like doped ceria-zirconia oxide sample of similar atomic fractions of the corresponding elements (Pt/PrSmCeZrO/YSZ) in methane dry reforming. The Pt+Ni/SmPrCeZr/YSZ nanocomposite catalyst is regarded to be the most effective on a per unit mass basis. Higher methane conversions and H2/CO ratios in the synthesis gas were obtained, while only minor differences were observed in the CO2 conversions.
AB - Methane dry reforming kinetics over the 1.2% Pt/80% Pr0.15Sm0.15Ce0.35Zr0.35Ox+10%NiO+10% YSZ catalyst (Pt+Ni/PrSmCeZrO/YSZ) has been assessed. First-order kinetics in methane was found for the forward reaction rate up to an equimolar methane/carbon dioxide feed ratio. The reaction rate was inhibited by adding methane beyond the stoichiometric value. A relatively constant zero reaction order towards CO2 can be applied when a CO2 excess of at least 1.5 over the stoichiometric value is employed. The existence of two different activation regimes is evident in Arrhenius plots with an inflection point at about 750°C. Kinetic parameters for the net rate of CH4 conversion over the Pt+Ni/PrSmCeZrO/YSZ composite catalyst were also determined by regression. The novel Pt+Ni/PrSmCeZrO/YSZ catalyst was benchmarked against a complex Pt-promoted fluorite-like doped ceria-zirconia oxide sample of similar atomic fractions of the corresponding elements (Pt/PrSmCeZrO/YSZ) in methane dry reforming. The Pt+Ni/SmPrCeZr/YSZ nanocomposite catalyst is regarded to be the most effective on a per unit mass basis. Higher methane conversions and H2/CO ratios in the synthesis gas were obtained, while only minor differences were observed in the CO2 conversions.
KW - Dry reforming
KW - Fluorite-like complex oxide catalyst
KW - Kinetics
KW - Methane
UR - http://www.scopus.com/inward/record.url?scp=84944707109&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2015.09.049
DO - 10.1016/j.apcatb.2015.09.049
M3 - Article
AN - SCOPUS:84944707109
VL - 182
SP - 513
EP - 524
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
SN - 0926-3373
ER -
ID: 25395991