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Thesis for degree: Licentiate of Engineering

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cathode are assumed to be similar to the case <strong>of</strong> the reactor bed. The aim <strong>of</strong> this case study is<br />

to examine whether the kinetics used <strong>for</strong> previous models [1] fulfill these criteria so no<br />

limiting effects occur <strong>for</strong> the heat and mass transport.<br />

The macroscale (2D) computational fluid dynamics (CFD) model <strong>of</strong> an intermediate<br />

temperature anode-supported SOFC operating on 30% pre-re<strong>for</strong>med natural gas is the base<br />

<strong>for</strong> the calculations per<strong>for</strong>med here. First, the criteria <strong>for</strong> the different domains are described<br />

and defined below. Then, the results <strong>of</strong> the analysis <strong>for</strong> the SOFC are presented in the next<br />

chapter.<br />

3.3.1 Interparticle transport<br />

The largest scale in this analysis is <strong>for</strong> the interparticle transport which is also sometimes<br />

called intrareactor scale because it applies to gradients within the reactor as a whole.<br />

Transport phenomena can occur both radially and axially within the reactor and these are hard<br />

to control and evaluate. For the SOFC the axial direction refers to the main flow direction (xdirection)<br />

and the radial direction refers to the direction normal to the main flow direction (ydirection).<br />

But if neglected, radial temperature gradients can <strong>for</strong>ce the reaction rates to be<br />

thousandfold greater <strong>for</strong> parts <strong>of</strong> the reactor <strong>of</strong>ten close to the axis [49]. For the SOFC this<br />

would occur in the anode and near the electrolyte close to the inlet <strong>of</strong> the cell and would mean<br />

a risk <strong>for</strong> disturbing “hot spots”. This can be checked by radial dispersion [50]:<br />

(3.38)<br />

where Bi R is the Biot number based on the reactor diameter, ΔH the enthalpy change <strong>of</strong><br />

reaction, r r the reaction rate, R o the reactor diameter, k e the thermal conductivity <strong>for</strong> the solid<br />

porous media, T w the temperature at the solid surface and γ the dimensionless activation<br />

energy. The axial dispersion is a less frequent limitation in a severe manner. Axial<br />

temperature gradients and axial conduction are possible to neglect if the length-to-particle<br />

diameter ratio is large enough (L/d p > 30) which is the case <strong>for</strong> SOFCs [50]. The criterion <strong>for</strong><br />

the limitation <strong>for</strong> the temperature gradient across the reactor diameter is defined as [49]:<br />

(3.39)<br />

where the parameters are the same as <strong>for</strong> equation (3.38) except the Biot number, R the gas<br />

constant and E a the activation energy.<br />

Mears [49] described an approach to adopt a differential reactor and this seems to be a very<br />

useful approach <strong>for</strong> the SOFC reactor beds. A differential reactor consists <strong>of</strong> different<br />

amounts <strong>of</strong> catalyst throughout the reactor bed to compensate <strong>for</strong> unfavorable effects such as<br />

extremely high reaction rates in parts <strong>of</strong> the reactor. For the SOFC one would wish to level<br />

out the reactions and the electricity generating action over the whole bed. This can be<br />

achieved by either increasing the amount <strong>of</strong> catalyst or to use finer particles to increase the<br />

reaction rate. However, the SOFC has contradicting needs <strong>for</strong> the reaction rates depending on<br />

whether the focus is on the methane steam re<strong>for</strong>ming reaction or electrochemical reactions.<br />

For the steam re<strong>for</strong>ming reaction, the reaction rate is very high at the inlet and then gradually<br />

decreases in the flow direction <strong>for</strong> the cell. But the reaction rate <strong>for</strong> the electrochemical<br />

reactions requires a higher reaction activity right at the inlet <strong>for</strong> a limited area which would<br />

increase if more catalyst material was provided or finer particles were present. By adjusting<br />

the reaction rate activity <strong>for</strong> its needs, severe effects <strong>of</strong> temperature or concentration gradients<br />

could be minimized.<br />

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