Date post: | 21-Dec-2015 |
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Acknowledgements
• Jonnie Bamforth (Leeds)
• Rita Tóth (Debrecen)
• Vilmos Gáspár (Debrecen)
• British Council/Hungarian Academy of Science
• ESF REACTOR programme
Flow Distributed Oscillations
• patterns without differential diffusion or flow
• Very simple reactor configuration:
plug-flow tubular reactor fed from CSTR
• reaction run under conditions so it is oscillatory in batch, but steady-state in CSTR
Kuznetsov, Andresen, Mosekilde, Dewel, Borckmans
Simple explanation
• CSTR ensures each “droplet” leaves with same “phase”
• Oscillations occur in each droplet at same time after leaving CSTR and, hence, at same place in PFR
Explains:
existence of stationary patterns
need for “oscillatory batch” reaction
BZ system with f = 0.17 cm s1
[BrO3] = 0.24 M, H+ = 0.15M
[MA] = 0.4 M, [Ferroin] = 7 104 M Images taken at 2 min intervals
• Doesn’t explain
critical flow velocity
nonlinear dependence of wavelength on flow velocity
other responses observed, especially the dynamics of pattern development
Analysis
• Oregonator model:
Has a uniform steady state uss, vss
)(
)()1(
12
2
qu
qufvuu
x
u
x
u
t
uP
vux
v
x
v
t
vP
2
2
Perturbation: u = U + uss, v = V + vss
linearised equations
Seek solutions of the form
VjUjx
U
x
U
t
UP 12112
2
VjUjx
V
x
V
t
VP 22212
2
U Aei x t ( ) V Bei x t ( )
Dispersion relation
2 2 3 4 2 2
) ( 2 2 2 ) , ( Tr i i Tr DP P P
0 Tri P
Tr = j11 + j22
= j11j22 – j12j21
2221 422)( TrTriP
Absolute to Convective Instability
Look for zero group velocity, i.e. find =0such that
gives
so
Setting Im(0)) = 0 gives AC
( )
0
0
012 i P
2221
21
0 4()( TrTri P
Bifurcation to Stationary Patterns
Required condition is = 0 with Im() = 0
Setting = 0 yields
So Im() = 0 gives critical flow velocity
0)(2 2234 PPP iTrTri
Tr
TrcrP 2
4 2
,
Initial Development of Stationary Pattern
• Oregonator model = 0.25f = 1.0q = 8 104
= 2
0.4 time units per frame
Experimental verification
BZ system with f = 0.17 cm s1
[BrO3] = 0.2 M,
H+ = 0.15M[MA] = 0.4 M, [Ferroin] = 7 104 M
Adjustment of wavelength to change in flow velocity
Oregonator model as before,
• Pattern already established
• now change from 2.0 to 4.0