International Journal of Engineering Research & Science (IJOER)

ISSN:[2395-6992]

[Vol-2, Issue-2, February- 2016]

Numerical Study of Microbial Depolymerization Process with the

Gradate School of Environmental and Life Science, Okayama University, Okayama, JAPAN
2
Center for Fiber and Textile Science, Kyoto Institute of Technology, Kyoto, Japan

AbstractComputational techniques are proposed for a numerical solution of an inverse problem that arises in a study of a
microbial depolymerization processes. The Newton-Raphson method in conjunction with the Newtons method is applied to
a time factor that involves three parameters. The Newton-Raphson method reduces a system of three equations for three
unknowns to a single variable equation, which is solved with the Newtons method. Those techniques were applied to a
microbial depolymerization process of polyethylene glycol. Introduction of experimental results into analysis leads to
simulation of a microbial depolymerization problem.
Keywords Newtons method, Newton-Raphson method, biodegradation,
simulation.

I.

polymer, mathematical model, numerical

INTRODUCTION

Petroleum-based polymers have been produced since the early part of the twentieth century. A large amount of those
xenobiotic compounds have been accumulated on the surface of the earth, and they are now sources for carbon dioxide
emission. Although those macromolecules had been nonexistent until they were invented, some of microorganisms are able
to utilize the carbon sources. Mechanisms of microbial depolymerization processes must be clarified for appropriate
assessment of the carbon cycle. Microbial depolymerization processes are categorized into exogenous type processes and
endogenous type processes. Monomer units are liberated one by one from terminals of molecules in an exogenous type
depolymerization process. Polymers degraded in exogenous type depolymerization processes include polyethylene (PE) and
polyethylene glycol (PEG). Unlike exogenous type depolymerization processes, primary factor of an endogenous type
depolymerization process is arbitrarily scission. Polymers degraded in endogenous type depolymerization processes include
polyvinyl alcohol (PVA) and polylactic acid (PLA).
A PE biodegradation process involves two primary factors, gradual weight reduction due to the -oxidation and direct
absorption by cells. A PE molecule liberates a two carbon unit from its terminal in one cycle of -oxidation and reduces in
size undergoing successive -oxidation processes until it becomes small enough to be absorbed directly into cells. A
mathematical model based on those factors was proposed for simulation of PE biodegradation processes [1 - 4].
Polyethylene glycol (PEG) is another polymer depolymerized in exogenous type depolymerization processes. The initial
step of liberation from a PEG molecule is oxidation of a terminal unit to produce an aldehyde, which is further oxidized to a
monocarboxylic acid. The oxidation is followed by the cleavage of the ether bond, and the molecule reduces by one glycol
unit [27]. Numerical techniques developed for PE biodegradation were applied for simulation of an exogenous type
depolymerization process of PEG [5]. Temporal factors of degradation rates were taken into consideration [6 - 8].
A mathematical model of endogenous type depolymerization processes was proposed for an enzymatic degradation process
of PVA [9, 10]. The model was applied to an enzymatic hydrolysis of polylactic acid (PLA), and degradabilities of PVA and
PLA were compared [11]. Temporal dependence of the degradation rate was taken into consideration for the
depolymerization process of PLA [14]. The model proposed for endogenous type depolymerization processes was
reformulated for exogenous type depolymerization processes of PEG [13] and PE [14]. Numerical techniques developed for
PE biodegradation were applied to an exogenous depolymerization process of PEG [15]. Temporal dependence of
degradability was taken into consideration for depolymerization processes of PEG [16 23, 25, 26].
The study on microbial depolymerization processes of PEG was continued. In previous studies, weight distributions of PEG
before and after cultivation of microbial consortium E1 were introduced into analysis, and techniques to evaluate parameters
for a time factor of degradation rate were proposed. In this study, those techniques were improved. The Newton-Raphson
method reduces a system of three equations with three unknowns to a single equation of one variable equation which is
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solved numerically by the Newton's method. Our techniques are illustrated with results obtained from application to weight
distributions before and after cultivation of Microbial consortium E1 for two days, four days, and seven days

II.

DESCRIPTION OF PROBLEMS IN ANALYSIS OF EXOGENOUS TYPE DEPOLYMERIZATION PROCESSES

Molecules of a single polymer all have the same chemical structure, while their molecular weight varies from one molecule
to another. In order to model a microbial depolymerization process, let t and M be the time and the molecular weight,

respectively, and let wt , M be the weight distribution with respect to the molecular weight M at time t , that is, the total
mass of polymer molecules for A M B is the integral

wt , M dM .
B

(1)

Let t be the microbial population at time t . The following system of equations was proposed in previous studies (cf.
[25]) under the assumption that the liberated amount distributes exponentially [24].

w
t M w cM K d K wt , K dK ,

(2)

d

,
k 1 h
dt
vt

(3)

where

cM Me M , d K

Function

e K

K 1 e K

vt is the residual in the culture medium at time t , that is,

which is approximated as the integral (1) for appropriate values of A and B . The microbial consortium E1 is incubated in a
culture medium where PEG 6000 was the sole carbon source. The weight distributions are obtained before and after
cultivation for two days, four days, and seven days. Table 1 shows approximate values of the residual PEG v0 , v2 , v4 ,
and v7 for A 103.2 , B 104.2 . The system of equations (2), (3) is associated with the initial condition

w0, M f 0 M ,

0 0 ,

(4)

Where f 0 M and 0 are the initial weight distribution and the initial microbial population, respectively. The system of the
equations (2), (3) and the initial condition (4) form an initial value problem. Given the initial weight distribution f 0 M , the
initial value problem (2), (3), (4) is solvable provided the molecular factor M and the initial microbial population 0 , and
the values of the parameters k and h are given. In what follows, techniques for determination of those unknowns are
described. Suppose that weight distributions at t t 0 , t t1 , t t 2 , and t t 3 are expressed with prescribed functions
f 0 M , f1 M , f 2 M , and f 3 M , respectively. Here t 0 0 and f 0 M is the initial weight distribution. A problem

posed in previous studies is to determine the values of the parameters 0 , k and h , which satisfy

wt1 , M f1 M , wt 2 , M f 2 M , wt3 , M f 3 M .

(5)

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Equation (2) involves t while equation (3) involves vt , the integral of wt , M with respect to M . In order to remove
the mutual dependence, consider the change of independent variables from

t to by

s ds .
t

(6)

Note that

d
t
dt

(7)

holds. Let

W , M wt , M , S t .
In view of the expression (7), equations (2) and (3) are converted to

W
M W cM K d K W , K dK ,
M

dS
S
1 h
,
d
vt

(8)

(9)

Respectively. Note that the equation (8) now involves only one of the unknown variables W , which makes the inverse
problem for the molecular factor M solvable, while the equation (2) involves two unknown variables w and .
Given the molecular factor of the degradation rate M and a weight distribution F1 M for T1 , equation (8) and the
initial condition

W T1 , M F1 M

(10)

form an initial value problem. Given an additional weight distribution F2 M for T2 , equation (8), the initial condition
(10), and the additional condition

W T1 , M F1 M

(11)

form an inverse problem for M , for which the solution of the initial value problem (8), (10) also satisfies the condition
(11). Techniques to solve the inverse problem were developed in the previous studies. In particular, the molecular factor
M was evaluated for T1 0 and T2 2 , for which F1 M and F2 M were the weight distributions of PEG after

cultivation of the microbial consortium E1 for two days and four days, respectively. Once M was obtained, the initial
value problem consisting of the equation (8) and the initial condition

W 01 , M f 0 M

(12)

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FIGURE 1: Transition of residual PEG for 010 based on the solution of the initial value problem (8), (12). The
initial value problem (8), (12) was solved numerically, and curve (, y()) was generated y V 100 ,

V 0

3 .2
4 .2
V W , M dM , A 10 and B 10 .

TABLE 1

Values of t and , and residual PEG before and after cultivation of microbial consortium E1 for two days, four days,
and seven days ( A 103.2 and B 104.2 ). The table shows the values of t , approximate values of , and approximate
values of the residual PEG (%) based on the conditions (5).

t
0.00000
2.00000
4.00000
7.00000

0.00000
0.51745
2.01635
7.21585

Residual PEG
(%)
100.00000

72.39508
26.59018
1.89424

was solved, and the residual PEG V as a function of ,

V W , M dM
B

was obtained ( A 103.2 and B 104.2 ).

(13)

Figure 1 shows the curve , V for 0 10 . Values of corresponding to

values of t were obtained by solving the equations V vt for t 0 , 2, 4, and 7 (Table 1). Table 1 shows that

t 2.0 , t 4.0 , and t 7.0 correspond to 0.51745, 2.01635, and 7.21585, respectively.
III.

NUMERICAL TECHNIQUES FOR EVALUATION OF PARAMETERS OF TIME FACTOR

The solution S of equation (9) with the initial value 0 depends not only on but also on 0 , k and h . Denote by

S S , 0 , k , h the solution of (9) which satisfies the initial condition S 0, 0 , k , h 0 . Let

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u , 0 , k , h

S q, 0 , k , h

[Vol-2, Issue-2, February- 2016]

dq .

In view of the expression (7), t u , 0 , k , h . Suppose that t1 , t 2 , and t3 correspond to 1 , 2 , and 3 according to the
change of variables (6), that is,

t i u i , 0 , k , h

i 1, 2, 3.

(14)

Let g i 0 , k , h u i , 0 , k , h ti , and consider the system of equations for the unknowns 0 , k and h obtained from
the conditions (14),

g i 0 , k , h 0

i 1, 2, 3.

(15)

In order to solve the system of equations (15), consider the first two equations

g1 0 , k , h 0 ,

g 2 0 , k , h 0

(16)

for a fixed non-negative value of h . System of equations (15) can be solved for 0 and k numerically by the NewtonRaphson method to generate functions h and h such that a solution of the system is given by 0 h , k h ,
that is, a sequence of approximate solutions 0,0 , k0 , 0,1 , k1 , 0, 2 , k2 , is generated by the recurrence formula
1

0,m1 0,m

g g 2 g 2 g1 g 2
g

g1 1 g 2 ,
k

0 k 0 k k

g g 2 g 2 g1

k m1 k m 1

0 k 0 k

(17)

g 2

g

g1 1 g 2 ,
0
0

m 0, 1, 2, ,

where the functions g1 and g 2 and their partial derivatives are evaluated at 0 0,n and k k n . Note that

g i
u

0 0

,
i

g i u

,
k k i

g i u

,
h h i

(18)

while the partial derivatives u / 0 , u / k , and u / h are the solutions of the initial value problems

d
d

u
1
S

,
2

S
0

d
d

1 S
u
,

2 k

d u
1 S
,

d h
S 2 h

u
0

0,

(19)

u
0,
k 0
u
0.
h 0

(20)

(21)

Partial derivatives S / 0 , S / k , and S / h are the solutions of the initial value problems

d
d

S
kh S

,
V 0
0

S
0

1,

(22)

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d S
hS kh S

1
,
d k
V V k

d
d

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S
0,
k 0

k
S
S

S h ,

h
V

(23)

S
0.
h 0

(24)

Those initial value problems are solved for the partial derivatives which appear in the recurrence formulas (17) [26].
Note that the system (16) leads to
1

g g
g g g g g g
h 1 2 2 1 2 1 1 2 ,
0 k 0 k k h h k

(25)

g1 g 2 g 2 g1 g 2 g1 g1 g 2

,

0 k 0 k 0 h 0 h

h
for 0 h and k h . Let

Z h g 3 h , h , h .

(26)

Once the solution 0 h , k h of the system (16) is obtained, the Newton's method can be applied to
Z h 0 ,

(27)

that is, a sequence of approximate solutions h0 , h1 , h2 , can be generated by

Z hn
,
Z hn

n 0, 1, 2, .

(28)

Note that
Z h

for 0 h and k h . Derivatives

g 3
g
g
3 3
0
k
h

and are given by the expressions (25), while the partial derivatives of g1 ,

g 2 , and g 3 with respect to 0 , k and h are given by expressions (18) - (24).

IV.

NUMERICAL RESULTS FROM ANALYSIS OF INVERSE PROBLEM FOR TIME FACTOR

Let V be the residual PEG obtained from a numerical solution of the initial value problem (8), (12), that is, V is the
function defined by the expression (13) for A 103.2 and B 104.2 . The system of equations (15) was solved numerically for
0 , k and h with the techniques described in the previous section. Table 2 shows the results from application of the
Newton-Raphson method to system (16) and the Newton's method to equation (27). Figure 2 shows the transition of the
residual PEG obtained from a numerical solution of the initial value problem (8), (9), (12) with S 0, 0 , k , h 0 . Figure 2
also shows the transition of residual PEG obtained from a numerical solution of the initial value problem (2), (3), (4) for the
values of the parameters 0 , k and h in the last row of table (2). The initial value problem (2), (3), (4) was solved
numerically using values of parameters 0 , k and h in the last row of table (2). Figure 3 shows the transition of the residual
PEG obtained from a numerical solution of (2), (3), (4).

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TABLE 2
Change of parameter values and iteration counts of the Newton-Raphson method and the Newton's method. The
table shows that hn 1 hn 10 12 for n 5 in the sequence generated by the Newton's method (28). It also shows that

0 , m 1

2
2
0,m k m1 k m 1012 for m 16 at each step of the Newton's method. Entries in the columns

0,n and k n are the last values of the Newton-Raphson iterations at the n th step of the Newton's method. The initial
value of each application of the Newton-Raphson method was fixed ( 0,0 0.2 , k 0 0.5 ).

n
0
1
2
3
4
5

hn 1
12.91011526876690
12.75353240846410
12.75316315092790
12.75316339202850
12.75316339186900
12.75316339186950

0, n

Count

16
16
16
16
16
16

0.14381126167661
0.14343204594116
0.14345256753083
0.14345261590947
0.14345261587788
0.14345261587790

kn
0.54194442446577
0.54498679389487
0.54482207592820
0.54482168762418
0.54482168787771
0.54482168787755

g 3 ( 0,n , k n , hn )
-0.20163026883843
0.01215719681922
0.00002849758473
-0.00000001860676
0.00000000001231
-0.00000000000004

FIGURE 2: Transition of residual PEG for seven days based on the initial value problem (8), (9), (12). The curve

u , 0 , k , h, y is shown y V 100 .

Function u , 0 , k , h was generated from a numerical solution of the

initial value problem (8), (9), (12) with the initial condition S 0, 0 , k , h 0 for the values of the parameters 0 , k
and h in the last raw of table 2.

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FIGURE 3: Transition of residual PEG for seven days based on the initial value problem (2), (3), (4). The curve

t, zt is shown zt vt 100 .

Function vt was generated from a numerical solution of the initial value

problem (2), (3), (4) for the values of the parameters 0 , k and h in the last raw of table 2.

Figure 1 shows that the residual PEG V may well be approximated by an exponential function. Suppose that V is a
solution of
dV
V ,
d

(29)

so that V V 0 e . Suppose that the value of is determined by the conditions

V 1 V1 ,

V 1 V2 ,

(30)

where V1 and V2 are the residual PEG at 1 and 2 , respectively, so that

logV2 logV1
.
2 1

Figure 4 shows the curve , e 100 . The figure also shows the curve , y (Figure 1). Parameters 0 , k and h
were evaluated for V V0e

with the techniques described in the previous section, where V0 is the residual PEG before

cultivation, that is,

V0 w0, M dM
B

A 10

3.2

, B 104.2 .

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B
FIGURE 4: Curve , e 100 . Curve , y is also shown y V 100 , V W , M dM , A 103.2

V 0

and B 104.2 .

TABLE 3
Change of parameter values and iteration counts of the Newton-Raphson method and the Newton's method for
V V0 e . The table shows that hn 1 hn 10 12 for n 5 in the sequence generated by the Newton's method (28).
It also shows that

0 , m 1

Entries in the columns

2
2
0,m k m1 k m 1012 for m 16 at each step of the Newton's method. .

0,n and k n are the last values of the Newton-Raphson iterations at the n th step of the

Newton's method. The initial value of each application of the Newton-Raphson method was fixed
( 0,0 0.2 , k 0 0.5 ).

hn 1
0
1
2
3
4
5

8.58671318397139
8.51606276891822
8.51591999712240
8.51592005463291
8.51592005460980
8.51592005460968

0, n

Count

16
16
16
16
16
16

0.14379681030420
0.14398144583988
0.14399064713205
0.14399066572345
0.14399066571597
0.14399066571597

kn
0.54208111099523
0.54059785942797
0.54052396031086
0.54052381099793
0.54052381105807
0.54052381105804

g 3 ( 0,n , k n , hn )
0.18837377402843
0.00856257414694
0.00001721986678
-0.00000000693634
0.00000000000279
0.00000000000001

Figure 5 shows the transition of the residual PEG obtained from a numerical solution of the initial value problem (8), (9),
(12) with S 0, 0 , k , h 0 and V V0e for the values of the parameters 0 , k and h in the last raw of table 3.

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FIGURE 5: Transition of residual PEG for seven days based on the initial value problem (8), (9), (12). The curve

u , 0 , k , h, y is shown y V 100,

V V0 e . Function u , 0 , k , h was generated from a

numerical solution of the initial value problem (8), (9), (12) with the initial condition S 0, 0 , k , h 0 for the values
V 0

of the parameters 0 , k and h in the last raw of table 3.

V.

CONCLUSION

Application of the Newton-Raphson method to the system (16) was demonstrated in a previous study, while the bisection
method was applied to the equation (27) [26]. The techniques were tested by application to model problem in which V
was a constant function. The techniques were also applied to an exponential function V e a b where the least square
approximation was applied to V based on weight distributions before and after cultivation of microbial consortium E1 for
one day, three days, five days, and nine days, and the values of the parameters 0 0.14345, k 1.5690 and h 9.3784
were obtained [26].
In this study, the application of the Newton's method to the equation (27) was illustrated. The techniques were applied to the
residual PEG V based on the weight distributions before and after cultivation of microbial consortium E1 for two days,
four days, and seven days. The values of the parameters 0 0.14345, k 0.54482 and h 12.75316 (Table 2) were
obtained. Values of 0 between numerical results in the previous study and this study are almost identical. However there
are notable differences in values of k and h .
Equations (16) and (27) were also solved for the solution of the equation (29) with the initial value V 0 , and the values of the
parameters 0 0.14399 , k 0.54052 and h 8.51592 (Table 3) were obtained. Difference in values of 0 and k
between shown in Table 2 and 3 is negligible. However there is a notable difference between the values of h shown in
Tables 2 and 3. Nevertheless, transitions of residual PEG shown in Figures 3 and 5 are indistinguishable, and equation (8)
may well be replaced with equation (29). In practical applications, there are cases where amounts of residual polymer is
available at discrete points in time instead of weight distributions. Techniques developed in this study will be applicable to
those cases.

ACKNOWLEDGEMENTS
The authors thank Ms. Y. Shimizu for her technical support. This work was supported by JSPS KAKENHI Grant Number
24540127.
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International Journal of Engineering Research & Science (IJOER)

ISSN:[2395-6992]

[Vol-2, Issue-2, February- 2016]

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