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Kinetics

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k1

B

k2

C

dC A

rA kC A (87)

dt

dC B dC B

rB1 kC A , rB 2 k2CB (88)

dt dt

dC B

For overall reaction: rB k1 C A k 2 C B (89)

dt

dC C dC B

rC k 2C B k1C A0 e k1t k 2 C B

dt dt

dC A dC B

rA k1C A k 2 C B k1C A0 e k1t

dt dt

C A dC t

C A0 C A 0 kdt

A

IF e k 2t

C

ln A k1t

C A0

dC B

e k 2t e k 2t k 2 C B k1C A0 e ( k2 k1 )t

dt

C A C A0 e k1t

dt

d k 2t

e C B k1C A0 e ( k 2 k1 ) t

e k2t C B

1

k 2 k1

k1C A0 e ( k 2 k1 )t M

At t = 0; CB = CB0

kC

C B 0 1 A0 M

k 2 k1

CB

k 2 k1

k1C A0 k1t

e e k2t C B 0 e k2t (90)

kC

M C B 0 1 A0 if CBO = 0

k 2 k1

k1C A0 e ( k 2 k1 ) t

e CB

k 2t kC

C B 0 1 A0 CB

k 2 k1

k1C A0 k1t

e e k 2t (91)

( k 2 k1 ) ( k 2 k1 )

dC C

rC k 2C B

dt

C B 0 C B CC

C B C B 0 CC

dC C

dt

k kC

k 2 C B 2 1 A0 e k1t e k 2t

k1 k 2

Revision 1: 2011

25

CC

e

t

k 2 k1 C A 0

dCC

k1t

e k 2t dt

CC 0

k1 k 2 0

CC

k 2 k1C A0 k1t

k1 k 2

e

e k 2t C C 0 (92)

dC A dC A

0; 0 k1C A0 e k1t

dt dt

e k1t 0 k1t ln 0

ln 0

t max (93)

k1

dC B k1C A0 k1t

0; CB (e e k 2 t )

dt k 2 k1

dC B kC

1 A0 (k1e k1t k 2 e k 2t ) 0

dt k 2 k1

k 2 e k2t k1e k1t

ln kk12

t max (94)

k 2 k1

dC C k 2 k 1C A 0

0; CC ( k1e k1t k 2 e k 2t ) 0

dt k 2 k1

ln kk12

t max (95)

k 2 k1

A

k1

B, A

k2

C

dC A dC B dC C

rA k 1C A k 2 C A rB k1C A rC k 2C A

dt dt dt

CA

dC A t dC B

C A0

CA

(k1 k 2 )dt

0 dt

k1C A0 e ( k1 k 2 )t

k 2 C A0

CC e ( k1 k 2 )t

( k1 k 2 )

CA k 1C A 0

ln (k1 k 2 )t CB e ( k1 k 2 )t

C A0 ( k1 k 2 )

Revision 1: 2011

26

C A C A0 e ( k1 k2 ) t (96-98)

r kC k

Sp B 1 A 1 (99)

rC k 2 C A k 2

k1

For elementary reaction: Sp (100)

k2

r R

For non-elementary reaction: Sp B 1 (101)

rC R2

A

k1

B

B

k2

A

dC A

rA k1C A k 2 C A (102)

dt

C A0 C B 0 C A C B CA

k 2 CT 0

k1 k 2

1 e ( k1 k 2 ) t C A0 e ( k1 k2 )t (103)

C B C A0 C B 0 C A

C B CT 0 C A

dC A

At equilibrium: 0 Conversion: XA = amount of A converted (%)

dt

C A0 C A

k 1C A k 2 C B XA 100 (102)

C A0

C Aeq k2

k eq (103)

C B eq k1

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27

A

k1

B A B

k2

BB

dC A

rA k 1C A k 2 C A C B

dt

(104)

Material Balance:

C A0 C A C B C B C A0 C A

dC A

k1C A k 2 C A (C A0 C A ) (105)

dt

A

k1

B A C

k2

BC

dC A

rA k 1C A k 2 C A C C

dt

(106)

Material Balance:

C A0 C C 0 C A C C C B

dC A

k1C A k 2 C A C C 0 (107)

dt

aA bB

Pr oducts

dC A

I. In terms of concentration: r A k C A C Ap C Bq (Eqtn A) - 108

dt

dC A

II. In terms of partial pressure: rA k PA PAp PBq (Eqtn B) - 109

dt

P PB

CA A (Eqtn C) - 110 CB (Eqtn D) - 111

RT RT

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28

PAp PBq

rA k C A (Eqtn E) - 112

( RT ) p q

Equate Eqtn B to E:

PAp PBq

k PA PAp PBq k C A (113)

( RT ) p q

Let p + q = n

kCA

k PA (114)

( RT ) n

III. In terms of mole fraction

dN A

rA k N A N Ap N Bq (Eqtn F) - 115

dt

PA = partial pressure of A at any time t

π = total pressure of system

NA = mole fraction of A

NB = mole fraction of B

PB = partial pressure of B at any time t

PA PB NA P

NA ; NB ; CA A

V RT

p q

P P

rA k C A C C k C A A B

p

A

q

B

RT RT

p q

P P

k N A N Ap N Bq k C A A B

RT RT

p q p q

P P P P

k N A A B kCA A B

RT RT

kNA kCA

pq (116)

( RT ) p q

pq n

k N A kCA let p + q = n k N A kCA (117-118)

RT RT

Revision 1: 2011

29

PROBLEM SOLVING

1. The initial rate of a second order reaction is 5.7 x 10 -7 gmole/L-s and the initial

concentration of the reactants is both 0.2 gmole/L. What is the specific reaction rate expressed

in units of hours-cu.ft./lbmole. Find kp and kN at 300C and 1 atm. Express the rate in terms of

other variables.

Given:

RA = 5.7x10-7 gmole / L –s 2A → Products

CA = 0.2 gmole/ L

Sol’n

-ra = kCACA2

KCA = _-rA_ = _-5.7 x 10-7 gmole / L – s_

CA2 (0.2 gmole / L) 2

KCA = - 1.425 x 10 -5 L / gmole – s

KCA = - 8.219 x 10 -1 ft3 / lbmole – hr

(RT)2 [(0.08205 _L - atm_) (30 + 273.15 K) ] 2

Gmole – K

KPA = - 2.3033 x 10 -8 gmole / L – atm 2- s

KPA = 2.98 x 10 -7 lbmole / ft3 – (PSI)2 – hr

KNA = KCA ( _π_)2 = (-1.425 x 10-1 L/gmole – s) [__1atm__]

RT (0.08205 _L- atm_)(30+274.15K)]2

KNA = - 2.3033 x 10-4 gmole / L – s

KNA = -298 x 10 -5 lbmole / ft3 –hr

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30

2NO + O2 → 2NO2

Is assumed to be taking place at constant volume. The initial concentrations of NO and O 2 are

2 lbmoles and 1 lbmole respectively. No NO2 present initially. Derive the rate reactions in

terms of the total pressure (π) of the system.

A

k1

B

k2

C

initially. How long does it take to reach a steady value if k 1 = 0.833 moles/m3-s and k2 =

0.767/s? What is the steady state value? CB = 1.0866 moles/m3

R

k1

F , k1 0.4m 3 / mole min R

k2

A, k 2 2.0 / min

(a) mean residence time, t;

(b) CF ;

(c) CA for a conversion of 90% of R.

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31

OBJECTIVES:

To know how temperature affects the rate of reaction through understanding of the

three theorems proposed.

To apply the theorems in solving for kinetics reaction rate constant.

ri f 1 (Temperatur e) f 2 (composition)

k f 2 (composition)

A. Arrhenius Equation

EA

k ko e RT (120)

where:

k = rate constant;

ko = Arrhenius constant, frequency factor, or pre-exponential factor;

EA = Arrhenius Energy of Activation, Cal / g-mol,

R = Universal constant, 1.987 Cal/g-mol K; and

T = Absolute temperature, K.

gives a good empirical description of the temperature dependence of the rate constant of an

elementary reaction. Both EA and ko are independent of temperature. This expression fits

experimental data well over wide temperature ranges and is strongly suggested from various

standpoints as being a reasonable first approximation of the true temperature dependency.

For a given k1 and T1 Equation 31 becomes

EA

k1 ko e RT1

Revision 1: 2011

32

Apply the natural logarithm to both sides of the equation and simplify

EA

ln k1 ln ko e RT1

EA

ln k1 ln ko ln e RT1

E

ln k1 ln ko A

RT1

EA

ln ko ln k1 (121)

RT1

EA

ln k2 ln ko e RT2

EA

ln k2 ln ko ln e RT2

EA

ln ko ln k2 (122)

RT2

EA E

ln k1 ln k 2 A (123)

RT1 RT2

Simplifying further will give us Equation 36 which is the working equation if there two

sets of rate constant (k) and temperature (T) are given.

E E

ln k2 ln k1 A A

RT1 RT2

k2 E A �1 1 �

ln � �

k1 R �T1 T2 �

k E �T T �

ln 2 A �2 1 � (124)

k1 R �T1T2 �

2. When more than two sets of rate constant (k) and temperature (T) are available:

EA

k ko e RT (125)

Applying the natural logarithm to both sides of Equation 37 and simplifying will give

E

ln k ln ko A (126)

RT

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EA

Equation 38 is an equation of a straight line where ln ko and are the intercept and the

R

slope of the line, respectively. The natural logarithm of k ( ln k ) is plotted against the

�1 �

reciprocal of temperature � �in Figure 1.

�T �

ln

k

Figure 2. ln k vs. 1/T

1/T

E n (ln k )( 1T ) ( 1T )( ln k )

m

n ( 1T ) ( 1T )

2 (127)

R 2

( ln k )( ( ) ) ( )( (ln k )( ))

1 2

T

1

T

1

T

y int ercept ln k 0 (128)

n ( ) ( )

2

1 2 1

T T

The fact that k goes to zero as T goes to zero tells us that there must be an energy barrier that

the reaction has to cross. When two molecules encounter, if they are to react they usually need

to meet with sufficient kinetic energy to allow their chemical bonds to be redistributed to form

products. If we follow the total energy of the two molecules as their reaction proceeds, the

energy reaches a maximum at the transition state, where the old bonds are half broken and the

new bonds are half made. The energy profile thus has a barrier to reaction: the height of this is

the activation energy EA.

The number of molecules that meet to form the transition state is the molecularity of the

reaction. The reaction profile shows the exergicity of the reaction (energy released on

formation of products, ΔE). Clearly the activation energy for the reverse reaction is E A + ΔE.

Catalysis involves providing a reaction pathway which has a smaller energy barrier to reaction

EA, and hence gives a faster reaction. Reactions with high activation energies are very

temperature sensitive; reaction with low activation energies are relatively temperature

insensitive. A given reaction is much more temperature-sensitive at low temperature that at

high temperature. From the Arrhenius law the frequency factor ko does not affect the

temperature sensitivity of a reaction.

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Transition State

EA

Reactants

E

Products

products in an elementary reaction.

For all but reactions involving two bare atoms, the relative orientations of the species that

meet in the transition state is important. For the simple reaction H + H2 � H2 + H, the lowest

energy reaction pathway goes through a linear transition state in which the partial bonds are of

o o

equal length at 0.95 A ( the normal bond length is 0.74 A ).

Revision 1: 2011

35

The activation energy rises steeply for other directions of approach of the H atom. This is a

simple example of the very general steric effect for species to react, they not only need to

have sufficient energy to overcome the activation energy barrier, but they also need to collide

in the right orientation. The simple graph of energy against reaction coordinate conceals the

true complexity of reactions, since even for collinear H + H 2 reaction the energy is a function

of two variables (the two H…H separations). In general the potential energy of reacting

species can be described as a surface in n dimensions; for H + H 2 this can be shown as a

contour map.

The explanation of the Arrhenius Law is now clearer. The pre-exponential factor ko is

determined by the frequency with which collisions with the right orientation happen (ko is

numerically equal to the number of collisions per second with the right orientation for reactant

EA

concentrations of 1 mol dm-3). The exponential term e RT is the fraction of those collision

which have energies (for motion along the line of centers) greater than or equal to E A; the

exponential character is a consequence of the Boltzmann distribution, which describes the

way that energy is distributed amongst randomly moving particles at thermal equilibrium. The

T dependence of the collision frequency is usually masked by the exponential term in the

Arrhenius equation.

Revision 1: 2011

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A

k1

R, R

k2

A, H r (129)

d (ln K ) H r

By Van’t Hoff equation: (130)

dt RT 2

Where: K K G R / A k1 / k 2

d ( ln k1 ) d (ln k 2 ) H r

(131)

dT dT RT 2

d (ln k1 ) E d (ln k 2 ) E

12 and 22 (132)

dT RT dT RT

E1 E 2 H r (133)

Collision theory views the rate to be governed by the number of energetic collisions between

reactants. What happens to the unstable intermediate is of no concern. It is simply assumed

that this intermediate breaks down rapidly enough into products so as not to influence the rate

of the over-all process.

ECT

k ko' T e RT (134)

where, k is the specific rate constant, ko’ is the collision theory constant, T is the temperature

(K), R is the universal constant (1.987 cal/g-mol K), and ECT is the collision theory activation

energy (cal/g-mol).

The collision theory states that the number of molecules formed per unit time per unit volume,

which is the rate, is equal to the number of collisions multiplied by a factor f.

z = number of collisions of A and B in cm3 of reaction mixture/sec

f = fraction of collision involving molecules with x’s activation energy

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M MB

z 2AB C A C B 8RT A (136)

M AM B

CA and CB = concentration of A and B; molecules/sec

R = universal gas law constant

R = kB N 0

kB = Boltzmann’s constant, 1.38 x 10-16 erg/K.

N0 = Avogadro’s Number (6.023 x 1023 molecules/gmoles)

Mi = molecular weight

M A M B 12

rA f 2AB C A C B (8RT ) (137)

M AM B

1

MA MB

2

k0e E /( RT )

C A C B f C A C B 8RT

2

AB

M AM B

f e E /( RT )

1

M MB

2

k0 2

AB

8RT A

M AM B

1

M MB

2

k 8R A T 2 e E /( RT )

2 1

AB (138)

M AM B

k T 2 e E /( RT )

1

(139)

4kT N2 4kT 2

Z AA A2 n A2 A2 CA (140)

MA 10 6 MA

= number of collisions of A with A/ (sec-cc)

M = (molecular weight)/N, mass of a molecule, gms

N = 6.023 x 1023 molecules/gm mole, Avogadro’s number

CA = concentration of A, gmoles/liter

nA = NCA/103, number of molecules of A/cc

k = R/N = 1.38 x 10-16 erg/K, Boltzmann constant

Revision 1: 2011

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2

B 1 1

Z AB A n A n B 8kT

2 MA MB

2

B N 2 1 1

A 6

8kT C A C B (141)

2 10 MA MB

The more energetic and violent collisions between molecules lead to reaction, or more

specifically, only those collisions that involve energies in excess of a given minimum energy

E lead to reaction. From the Maxwell distribution law of molecular energies the fraction of all

bimolecular collisions that involve energies in excess of this minimum energy is given

approximately by

e-E/(RT)

col is onrate,

involvingenergies

moles/(liter)(sec)inexces of E

rA

1 dN A

V dt

kC A C B

1000 E /( RT )

Z AB e

N

2

B N 1 1 E /( RT )

A 3

8kT e C AC B

2 10 MA MB (142)

ECT

k1

ko' e RT1

T1

k1 E

ln ln ko'

T1 RT1

k E

ln ko' ln CT (143)

T1 RT1

Similarly for k2 and T2

Revision 1: 2011

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k2 E

ln ln ko' CT

T2 RT2

k2 E

ln ko' ln CT (144)

T2 RT2

Equating Equations 53 and 54

k2 E k E

ln CT ln 1 CT

T2 RT2 T1 RT1

k2 k E E

ln ln 1

T2 T1 RT1 RT2

�k2 �

�T � �

ln � 2 � E �T2 T1 �

�

� k1 � R �T1T2 �

�T �

� 1 �

�k2 T1 � ECT � T2 T1 �

ln �

�k �

� � � (145)

�1 T2 � R �T2T1 �

Equation 55 is used to determine the activation energy (ECT) if two sets of rate constants (k)

and temperature (T) are given.

ECT

k ko' T e RT

E

k CT

ko' e RT

T

Applying natural logarithm to both sides of the equation, then simplify will result into an

equation of a straight line.

k E

ln ln ko' CT

T RT

k 1

The plot of ln vs T is shown in Figure 5.

T

�k �

ln � �

�T �

1/T

Chemical Reaction Engineering and Kinetics Compiled by Mary Rose F. Persincula

Revision 1: 2011

40

�k �

Figure 5. Plot of ln � �as a function of (1/T) for the determination of

�T �

activation energy (ECT) and constant (ko’).

Transition-state theory views the reaction rate to be governed by the rate of decomposition of

intermediate. The rate of formation of intermediate is assumed to be so rapid that it is present

in equilibrium concentrations at all times. The governing equation is given Equation 56.

E ACT

k k o Te

" RT (146)

where, k is the specific rate constant, ko” is the activated complex theory constant, T is the

temperature (K), R is the universal constant (1.987 cal/g-mol K), and EACT is the activation

energy (cal/g-mol).

Reactants combining to form unstable intermediates called activated complexes which then

decomposes spontaneously into products. It assumes in addition that an equilibrium exists

between reactants and activated complex at all times and that the rate of decomposition of

complex is the same for all reactants and is given by kT/h where k is the Boltzmann constant

and h = 6.63 x 10-27 erg-sec is the Planck constant.

For k1 and T1

E ACT

k1 k T e

"

o 1

RT1

E ACT

k1

ko"e RT1

T1

E ACT

�k �

ln �1 � ln ko" ln e RT1

�T1 �

�k � E

ln ko" ln �1 � ACT (147)

�T1 � RT1

similarly for k2 and T2

�k � E ACT

ln ko" ln � 2 � (148)

�T2 � RT2

Revision 1: 2011

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�k ��T � E T T �

�

ln �2 ��1 � ACT �2 1 � (149)

�k1 ��

T2 � R �T2T1 �

E ACT

k

ko" e RT

T

E ACT

k

ln ln ko e RT''

T

�k � E

ln � � ln ko" ACT (150)

�T � RT

�k � 1

The Plot ln � �vs is shown in Figure 5.

�T � T

�k �

ln � �

�T �

�k � 1/T

ln

Figure 5. Plot of � �as a function of (1/T) for the determination of

�T �

activation energy (EACT) and constant (ko”).

with low activation energies are relatively temperature-insensitive.

2. A given reaction is much more temperature-sensitive at low temperature than at

high temperature.

3. From the Arrhenius law the frequency factor k0 does not affect the temperature

sensitivity of a reaction.

Revision 1: 2011

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Revision 1: 2011

43

PROBLEMS

1. At temperature 320F and 680F the standard rate of reaction are 2.46 and 47.5 sec -1

respectively. Determine the activation energy and the frequency factor.

Given :

T1 = 320F = 492 0R 1.987 cal / gmol – K

T2 = 680F = 5280R 1.987 BTU / lbmol – 0R

K1 = 2.46 sec -1

K2 = 47.5 sec -1

Req’d : EA and ko

Sol’n : ln _k2_ = _EA_ [ _T2 – T1_]

K1 R T1T2

Ln _47.5_ = _EA_ [ _528 – 492_ ]

2.46 = 1.987 (492)(528)

__ EA = 42,449.19759 BTU / lbmol

K1 = k2 e –E / RT

-42449.19759 / [ (1.987)(492)]

1.46 = ko e

Ko = 1.7731 x 10 19 sec -1

Using Collision Theoy

k1 = ko T11/2 e-Ect/RT1

ln __k1__ = ln ko - _ECT_ . _1_

T11/2 R T1

ln __k2__ = ln ko - _ECT_ . _1_

T21/2 R T2

ln __k1 T21/2__ = - _ECT _ [ _1_ - _1_ ]

k2 T11/2 R [ T1 T2 ]

ln _k1_ + _1_ ln _T2_ = - _ECT _ [ _T2 – T1_ ]

k2 2 T1 R [ T 1 T2 ]

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k2 R [ T 1 T2 ]

ln _2.46_ = - __ECT__ [ _528 – 492_ ]

47.5 1.987 [ (492)(528) ]

ECT = 41,942.93347 BTU / lbmole

2. Data on the effect of temperature on the reaction between ethanol and acetic acid catalyzed

by a cation-exchange resin were obtained by Soletan and Ukete

T, deg C 30 40 50 60 70

k, L/mole-hr 0.5 1.1 2.2 4.0 6.0

Solution:

m = __n∑XY – (∑X)(∑Y)__ y-int = __∑Y∑X2 - ∑ - ∑X∑XY__

n∑X2 - (∑X)2 n∑X2 - (∑X)2

Arrhenius:

k = koe-Ea/RT

ln k = ln ko – _EA_ [_1_]

R [ T ]

X 1/T (x103) 3.2987 3.1934 3.0945 3.0017 2.9142

Y ln k -0.6931 0.0953 0.7885 1.3863 1.7918

XY (x103) -2.2863 0.3043 2.4400 4.1613 5.2217

X2 (x105 1.0881 1.0198 0.9576 0.9010 0.8493

R 5(4.8158x10-5) – (15.5025x10-3)2

EA = 12973.9836 cal/gmole-K

20.9183 = y-int = ln ko

Chemical Reaction Engineering and Kinetics Compiled by Mary Rose F. Persincula

Revision 1: 2011

45

= _(3.3688)(4.8158x10-5) – (15.5025x10-3)(9.841x10-3)

5(4.8158x10-5) – (15.5025x10-3)2

ko = 1.2153x109 L/mole-hr

3. Determine the activation energy and the frequency factor from the following

data:

T(deg C) 0 100

k (/min) 0.001 0.05

(a) Use Arrhenius equation

(b) Transition state theory

(c) What is the % difference between the time activation energies in (a) and (b)

(d) Calculate the value of k at 10000C using (a) and (b). What is the % difference

between the two k at this temperature?

chloride to give chlorobenzene and nitrogen. Use the following information for the

first order reaction. (Use Arrhenius equation). Answer: E = 123 753.263 J/gmole

k(s-1) 0.00043 0.00103 0.00180 0.00355 0.00717

Revision 1: 2011

46

Sample Problems

Chemical Reaction Engineering and Kinetics

Directions: Solve the problems completely. Show your solutions in a neat and organized way

on the answer sheets provided. Round off your answer to four decimal places. Your solution

will be graded according to how the problem is solved.

R B k2 = 6 min-1

M is the desired product, B and F are foul pollutants that are expensive to get rid of.

a. Derive the rate law expressions for each species. (5 points)

b. Determine the time in seconds, to achieve 90% conversion of R (XR) for a feed of 3.0

lbmol/ft3. (20 points)

2. (10 points) The time required for one-half of the reactant to disappear is called the half-life

of the reaction.

a. Find the half life of the reaction A B with k = 0.5 mol/L-min and CA0 = 15

M. (5 points)

b. Find the half life of the reaction A B with k = 1 /min and CA0 = 15 M. (5

points)

3. For the reaction, A R, assumed to be first order in both forward and backward

reactions, the initial concentrations of A and R are 3M and zero respectively. Ten minutes

after, the conversion of A is 10%. After a long time, the concentration of A is 30% of the

initial concentration. Predict the conversion of A after 20 minutes.

4. A ten minute experimental run shows that 75% of liquid reactant is converted to product by

a ½ order rate. What would be the fraction converted in a half-hour run?

enzymes

A R -rA = 200 CA CEO mol

2 + CA L-min

If we introduce enzyme (CEO = 0.001 mol/L) and reactant (CAO = 10 mol/L) into a

batch reactor and let the reaction proceed, find the time needed for the concentration

of reactant to drop to 0.025 mol/L. Note that the concentration of enzyme remains

unchanged during the reaction.

Revision 1: 2011

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