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Partial oxidation of methane over Ni0/La2O3 bifunctional catalyst II: Global kinetics of methane total oxidation, dry reforming and partial oxidation

Paper ID Volume ID Publish Year Pages File Format Full-Text
45569 46416 2015 10 PDF Available
Title
Partial oxidation of methane over Ni0/La2O3 bifunctional catalyst II: Global kinetics of methane total oxidation, dry reforming and partial oxidation
Abstract

•The global Arrhenius equation was established for DR, TO and POM.•Ea of DR, TO and POM were 87.8, 116.4 and 112.8 kJ mol−1, respectively.•At 1073 K, kDR=69.3 {(mol m−3)1−α s−1}≫kTO=12.4 {(mol m−3)1−(γ+δ) s−1}kDR=69.3 {(mol m−3)1−α s−1}≫kTO=12.4 {(mol m−3)1−(γ+δ) s−1}; (kSR ≈ kDR).•Methane TO reaction is the rate determining cycle (rdc) of POM reaction (rPOM0=2rTO0 with kPOM ≈ 2kTO).

The global kinetics (power rate law) of methane total oxidation (TO) over La2O3 catalyst was performed at 773, 823 and 873 K. The global kinetics of methane dry reforming (DR) at 648, 673, 698 and 723 K and partial oxidation (POM) at 993, 1013, 1023 and 1053 K were conducted over Ni0/La2O3 catalyst. The initial rate method and isolation method were used to determine initial rates, rate constants, and partial orders to reactants and establish the Arrhenius equations for TO, DR, POM. The experimental apparent activation energies were 87.8, 116.4 and 112.8 kJ mol−1 for DR, TO and POM, respectively. For TO, the reaction order to CH4 was varying with conversion whereas that to O2 was zero. For DR, the reaction order to CH4 was constant, whereas that to CO2 was dependent on the concentration of CO2. The values of rate constants revealed the following order: kDR ≫ kPOM, kTO. It was found that the rate constant of POM reaction is linked to that of methane TO: kPOM ≈ 2kTO. The catalytic cycle of methane TO is the “rate determining cycle” (rdc) of the POM process.

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Keywords
POM; Global kinetics; Power rate law; Nickel; La2O3
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Partial oxidation of methane over Ni0/La2O3 bifunctional catalyst II: Global kinetics of methane total oxidation, dry reforming and partial oxidation
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 165, April 2015, Pages 389–398
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
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Price was $35.95
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