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BZ Reaction

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An Overview

By Melody Dodd

10 Dec. 2010

A Brief History of Chemical Oscillators

• Have only been recognized as mainstream

science since the 1960s.

progressed in one direction (monotonically) to

equilibrium.

A Brief History of Chemical Oscillators

• First oscillating reaction

discovered around 1950 by Boris

Pavlovich Belousov.

acidified bromate and ceric ions

oscillated from colorless to yellow

for up to an hour.

A Brief History of Chemical Oscillators

• Belousov’s work ill-received by scientific community.

contributions.

community to the validity of chemical oscillators.

Belousov-Zhabotinsky (BZ) Reaction.

A Brief History of Chemical Oscillators

• Today, many chemical systems are known to

oscillate.

to describe the BZ reaction.

▫ Brusselator

▫ Oregonator

remains a mystery.

Background: Chemical Kinetics

domain and are in motion.

A B C.

Background: Chemical Kinetics

decrease at the same rate, and the rate of change

of C will be the negative of this rate.

Background: Chemical Kinetics

• We can express the rate of change of concentrations

of A, B, and C as a dynamical system:

A r

B r

C r

• Intuitively, the reaction rate r depends on the

concentrations of A and B.

Background: Chemical Kinetics

r kAB

experimentally.

Background: Chemical Kinetics

• We will now extend this idea to more

complicated reactions. Consider

A B C D.

The constants , , , 0 are called the

stoichiometric coefficients of the reaction.

products.

Background: Chemical Kinetics

• We can derive a dynamical system for this

reaction using the Law of Mass Action.

1) The reaction rate r is proportional to the product

of the reactant concentrations, with each

concentration raised to the power equal to its

respective stoichiometric coefficient.

r kA B

Background: Chemical Kinetics

2) The rate of change of the concentration of each

species in the reaction is the product of its

stoichiometric coefficient with the rate of the

reaction, adjusted for sign (+ if product, - if

reactant)

A r

B r

C r

D r

Background: Chemical Kinetics

• Thus we arrive at the dynamical system

A k A B

B k A B

C kA B

D k A B .

With known initial concentrations

Modeling The BZ Reaction

• There are many variations on the BZ reaction recipe.

the following:

Solution Composition

Solution A 0.23M Potassium bromate

Solution B 0.31M Malonic acid,

0.059M Potassium bromide

Solution C 0.019M Cerium(IV) ammonium nitrate,

2.7M Sulfuric acid

Ferroin Indicator Solution

Modeling The BZ Reaction

• However, our analysis will concern the

Oregonator, which is based on a slightly

different recipe.

model of the BZ Reaction.

complicated; some models have as many as 80

steps and 26 variable species concentrations.

Modeling The BZ Reaction

• Let

be determined empirically).

Modeling The BZ Reaction

• Using the Law of Mass Action, we can derive the

following dynamical system:

known.

Modeling The BZ Reaction

• Using nondimensionalization and some

simplifying assumptions, we can reduce the

system to:

• Note that

Mathematical Analysis

2

• Taking f , q 8 10 4

, 4 10 2

(based on

3

empirical data using typical initial concentrations) yields

dx 50 1 1250 x

25 x(1 x) z

d 3 1 1250 x

dz

x z.

d

dx dz

0, 0.

d d

Mathematical Analysis

• We can graph the

nullclines and use test

points to find flow

directions.

positive fixed point

( x* , z * ).

fixed point will exist for

any f , q 0

Mathematical Analysis

• Plotting a few

trajectories reveals a

stable limit cycle.

point is clearly

unstable.

Mathematical Analysis

• A view of one

trajectory with initial

conditions close to

(0,0).

Mathematical Analysis

• In fact, this system exhibits relaxation oscillations.

Mathematical Analysis

• Question: What effect does varying initial

concentrations have on the limit cycle?

portrait that occurs as the real parts of eigenvalues of the

Jacobian matrix for the system (evaluated at a fixed

point) change from negative to positive.

will exist only for certain values of f and ε.

Mathematical Analysis

• For example, if we

increase ε to 0.6 (and

keep q and f the

same) then the limit

cycle vanishes.

point is now stable.

Mathematical Analysis

What values of ε and f will produce oscillations?

* *

( x , z

dx dz

solving the system d

0,

d

0 to obtain

x*

1

2

1 f q

f 2 (1 q) 2 f (6q 2) , z* x * .

Mathematical Analysis

2. Compute the Jacobian matrix for the system,

evaluated at the fixed point:

1 2 fx *q f (q x* )

1 2 x

*

* .

J (x , z )

* *

(q x )

* 2

(q x )

1 1

Mathematical Analysis

3. The critical value for ε will occur when the real

part of the eigenvalues for the Jacobian matrix

are equal to zero. This means the trace of the

Jacobian will be zero.

1 2 fx *

q

trace ( J ) 1 2 x

*

0

* 2

(q x )

*

2 fx q

1 2x *

(q x )

* 2

Mathematical Analysis

4. We can graph this result in the ε-f plane to

obtain a region in which oscillations will occur.

References

▫ Gray, Casey R, An Analysis of the Belousov-

Zhabotinskii Reaction.

▫ Holmes, M.H., Introduction to the Foundations

of Applied Mathematics.

▫ Strogatz, Steven H., Nonlinear Dynamics and

Chaos.

▫ Winfree, A.T., The Prehistory of the Belousov-

Zhabotinsky Oscillator.

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