The methanation of CO₂ was investigated over a wide range of partial pressures of products and reactants using a gradientless, spinning-basket reactor operated in batch mode. The rate and selectivity of CO₂ methanation, using a 12 wt% Ni/γ-Al₂O₃ catalyst, were explored at temperatures 453 – 483 K and pressures up to 20 bar. The rate was found to increase with increasing partial pressures of H₂ and CO₂ when the partial pressures of these reactants were low; however, the rate of reaction was found to be insensitive to changes in the partial pressures of H₂ and CO₂ when their partial pressures were high. A convenient method of determining the effect of H₂O on the rate of reaction was also developed using the batch reactor and the inhibitory effect of H₂O on CO₂ methanation was quantified. The kinetic measurements were compared with a mathematical model of the reactor, in which different kinetic expressions were explored. The kinetics of the reaction were found to be consistent with a mechanism in which adsorbed CO₂ dissociated to adsorbed CO and O on the surface of the catalyst with the rate-limiting step being the subsequent dissociation of adsorbed CO.JYL was funded by the Cambridge International Scholarship Scheme. The Cambridge Philosophical Society, the Lundgren Research Award and Corpus Christi College are also gratefully thanked for contributing to the support of his PhD studies.This is the author accepted manuscript. The final version is available from Elsevier via http://dx.doi.org/10.1016/j.ces.2015.10.02
