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J Phys Chem A ; 119(6): 943-51, 2015 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-25626014

RESUMO

Experiments to measure the hydrogen uptake kinetics of DEB getter/Pd catalyst/activated carbon pellets have been performed under isothermal isobaric conditions. The extracted kinetics were then used to predict the performance of the getter pellets under different temperatures and pressures, including nonisobaric situations. For isothermal isobaric uptake at higher H2 pressure (666.6-2666.5 Pa), H2 solubility in the getter matrix is responsible for the uptake observed up to a 40-60% reacted fraction. Once the hydrogenated product becomes thicker, the diffusions of the reactants (atomic hydrogen and getter molecules) toward the reaction front become the rate limiting step. However, in a dynamic but very low H2 pressure, encountered in many vacuum electronic applications, the hydrogen spillover effect, over micrometer scale, becomes the dominant reaction mechanism. Despite such a complex dependence of the rate limiting mechanisms on the experimental environment, there is good agreement between kinetic prediction models and experiments. The investigation also reveals that the ultimate uptake capacity in the getter pellets scales inversely with the free volume of the vacuum vessel in which the DEB getter pellets are used, and that DEB getter pellets' performance greatly deteriorates during the final 10-15% capacity (as evidenced by the sharp bend in the slopes of the reacted fraction vs time curves at 85-90% reacted fraction).

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