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**Hongqing Cao', Jingxian Yuz ,Lishan Kang'
**

$ate Key Laboratory of Software Engineering; Wuhan University, Wuhan 430072, China -email: (jxyu, kang)@whu,edu.cn 1 -Depanment of Chemistry, Wuhan University, Wuhan 430072, China email: jxyu@whu.edu.cn least.square method [3][41. But Some problems exist in using this method, like the sensitivity to initial values, the difficulty to compute the partial derivative expression of each parameter for some complex circuits and the great likelihwd to trap into local optima. In view of all above analysis, we consider that the most desirable way to analyze electrochemical impedance data is to build the equivalent circuit model automatically as well as optimize the component parameters simultaneously by using some intelligent approach. Hence this paper proposes a hybrid evolutionary modeling algorithm (HEMA) to approach this modeling task. Its main idea is to embed a genetic algorithm (CA) in gene expression programming (GEP) where GEP is employed to discover and optimize the structure of a circuit, while the CA is employed to optimize the parameters of all the electric components contained in the circuit.

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Abstract- This paper proposes an evolutionary approach to build the equivalent circuit model for electrochemical impedance spectroscopy. It works by using a hybrid evolutionary modeling algorithm (HEMA) whose main idea is tn embed a genetic algorithm (GA) in gene expression programming (GEP) where GEP is employed to discoverand optimize the structure of a circuit, while the GA is employed to optimize the parameters of all the electric components contained in the circuit. By running the HEMA, the computer can automatically find suitable circuit structures as well as optimize the component parameters simultaneously. Compared with most available methods, it has the advantages of automation . of modeling process, great diversity of model,structnres, high stability and efficiency of parameter optimization.

1 Introduction .

. . , . With ths development of electrochemical measurement technique, the acquisition of impedance data has become much easier than before. On the contrary, how to analyze and interpret those data is considered as a complicated and arduous task. Usually the interpretation of electrochemical impedance data includes three steps. First an equivalent circuit model for the examined system is built based on the measursd electrochemical impedance spectroscopy and relevant electrochemical knowledge. Second the parameter values of all components contained in the circuit are determined by using some curve-fitting methods. Finally some lanetic parameters in the electrode, reaction are calculated according to the circuit structure and the component parameters [I]. Among those, how to build a suitable model is the most crucial step. Among the available modeling software for equivalent circuits a1 present, the EQUIVCRT software developed by Boukamp [ 2 ] is applied most widely. However the EQUlVCRT software. requires the users to have abundant electrochemical professional knowledge and research experience, which limits its application range in some degree. As for the second step, people have done much work in this field. The most popular approach adopted by people to fit the impedance datais the complex non-linear

**2 Hybrid Evolutionary Modeling Algorithm
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Gene Expression Programming (GEP) is a linear genetic programming (GP) [5-71 with fixad length invented by Ferreira [8][9] in 2001. It is the natural combination of chromosomes of GP and GA [IO] in which the genotype and the phenotype are separated. In GEP the individuals are encoded as symbolic strings of fixed length (genotype) which are then expressed as non-linear expression trees (ETS) of different sizes and shapes (phenotype). In comparison with GP, the most advantage of GEP lies in that it allows the modification of the genome using any genetic operator without restrictions, producing always syntactically correct programs. But it has a major drawback in GEP, namely the inconvenience to handle numerical constants [9]. While for our case, when building an equivalent circuit model for electrochemical impedance, it involves not only the structure of the circuit, but also the parameters of all electric components contained in the circuit. Moreover the electrochemical impedance of a circuit is rather sensitive to the values of those parameters. Hence it is expected to achieve desirable results if we can deal with those parameters separately. Based on all above considerations, we propose a hybrid evolutionary modeling algorithm (HEMA) to approach the

0-7803-7804-0 /03/$17.00 B 2003 E E E

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and is evaluated by the equation: t=h(k-l)t I (1) As far as the equivalent circuit for electrochemical impedance is concerned. and all the new individuals produced by mutation are structurally correct programs. whereas the length of the tail I is a function of h and the number of arguments of the function with more arguments k. The head contains symbols that represent both functions and terminals. each gene has an effective coding segment (ECS) whose length equals to the number of nodes in the binary tree. When mapping a GEP gene into a circuit. r:=t+1. the correspondent circuit can he obtained easily.2 Genetic Operators In the HEMA. we use two kinds of crossover: one-pint crossover and two-point crossover and two kinds of mutation are adopted as well: multi-point mutation and segment-insenion mutation. the length of the segment and the insertion point.3n)C(ZUF1C~2~C(4~)CPE~lO~. in the tails.modeling task of the equivalent circuit for electrochemical impedance.O. For example. capacitors (C) and inductors (L). then r = 5 . In this way. while the GA is employed to optimize the parameters of all. For distinction. the structural organization of chromosomes is remained intact. Using GEP 2. In segment-insertion mutation a segment is randomly chosen throughout the parent chromosome.O 2) It can be convened into a tree structure shown in Fig. Its main idea is to embed a GA in GEP where GEP is employed to discover and optimize the structure of a circuit.chromosome as the mutation points. In the heads. despite its fixed length. if we'chose an h = 4. I(b). and the two possible ways to connect them are parallel and series. as linear symbolic strings of fixed length. we first convert it into a binary tree stmture of GP by following some rules descrikd in Ref. Thus we define the set of terminals T = {R. -1 where + and . Each gene is composed of a head and a tail. C . constant phase elements CPE(w. One such gene is shown Fig. For each problem. In multi-point mutation multiple points are randomly chosen from the ECS of the parent. The structure of the HEMA can be described as follows: Procedure HEMA begin input observed data of electrochemical impedance. 1 The binary tree structure of GEP gene (a) and h e correpondenicircuit (bj 2. initialize the circuit population. n). CPE. the possible electric components include resistors (R). [9]. while ( I < MAXGEP) do begin structure optimization process of circuit models using G E P parameter optimization process of electric components using GA. Thus the length of the gene is 4 + 5 = 9. 1:=0 below: -+R~50~~-L~82mH~R~O. According to the binary tree.1.1 Representation of Chromosomes The chromosomes in GEP are represented. end 21 Structure Optimization Pmcess of Circuit Models . Obviously in this case. whereas the tail contains only terminals. terminals can only change into terminals.the electric components contained in the circuit. any symbol can change into another (function or terminal). ](a) which corresponds to a circuit illustrated in Fig. k 2 . 1820 . except the first position. A copy of the segment is made and inserted at any position in the head of the chromosome. end output the best circuit model. the length of the bead h is chosen. So.represent the series connection and the parallel connection respectively.1. LJ and the set of functions F = {+. the ECS of each gene is underlined and the tail of a gene is shown in bold. This operator involves in the selections of the start of the segment.

experiments. and therefore all the new individuals created by.1.3 Calculation of Fitness Values As the electrochemical impedance of a circuit consists of a real part and an imaginary part.2 Parameter Optimization Process of Electric Components Using GA This parameter optimization process is done for each individual in the current circuit population.j . we first assign the parameter values in P to the correspondent components in the GEP parent chromosome one by one and then follow the same procedure in Section 2.e...e. L ) ( i :I-k). z2 When calculating the fitness value of an individual. m is the number of input frequencies. C(0-0. the better the individual.<. . in GA population. w .(2) based on those fitting values.. Suppose there are k parameters in total. ~ a.001F) and L(0-IH). on the one hand. = (p. f. We first determine the total number of the parameters to be optimized according to the number of terminals (i. p 2 . whereas the insertion point can only be chosen from-the head except the first element and the ECS of the chromosome. Similarly 2. we start 0-7803-7804-0 1031$17. Thus the fithess function. 2. Each pi has its own range of definition in terms of the component it 'corresponds to. 1 (c) the impedance of a capacitor: . Obviously. electric components) in the ECS of the individual gene and their types.5. P. Each time we randomly select M different individuals from the old population (M>2) denoted as P. is defined by the following equation: from the bottom level of the tree and figure out the electrochemical impedance of all branch circuits by using the formulae described above.. i. despite the insertion. Thus. It adopts a novel crossover operator which performs by the non-convex combination of multiple parents.p r ) ( i : l . The algorithm to do the parameter optimization in the HEMA is a genetic algorithm based on the subspace search. but on the other hand. the number . p 2 . If any parameter in P. we predefine the ranges of these parameters as R(O-IOOQ). Afterwards we trace back upward to access the tree level by level until the total impedance' of the whole equivalent circuit is achieved. (b) the impedance of a constant phase element CPE(w. Finally we can calculate the fitness value of p by using Eq.. + Z2. When the components are series-connected or.'.p X ) where p . in GEP population we first convert it into the correspondent tree structure. parallel-connected. n): When I I is 0. C .1. This value is just the fitting value of the electrochemical impedance for p under the given frequency f ." are the correspondent fitting values. Accordingly produce M random coefficients where 2..1. namely the real part and the imaginary part. the tail of the parent chromosome remains unchanged after insertion.. Then each individual in the parameter population. Py where P.. are and the imaginary part of the electrochemical impedance under a given frequency. 5 6 ( a < 0 .The former two can be chosen randomly. a segment with as many symbols as the inserted segment is deleted at the end of the head of the parent chromosome. 2@. The formulae for calculating the electrochemical impedance of each electric component are listed as follows: (a) the impedance of a resistor: R. Pne.3 to figure out the fitness value of I l l (b) Z1-22 parallel connection: ..and 2. the inserted segment becomes duplicated. P2. ~ ( R . n(0-I).of data points.= -+ z 2 . n . Then for each input frequency f . a one-dimensional line vector written in the form of P = b . the structural organization of chromosomes is maintained. is encoded as an ordered set of k floating numbers. P. is produced by the non-convex linear combination of those M individuals: 2nfc (d) the impedance of an inductor: . the equation is the Warburg impedance caused by the semi-infinite diffusion process.-Z? series connection: Z = Z. By following the same procedure.' and Z ? the actual values of the real part . When calculating the fitness value of an individual. which satisfies a < a. That is. we can calculate the sum of the least-square errors of those two parts as the fitness value of an individual.. then abandon this invalid individual and recreate a new one by reproducing a new set of ai and following the Eq.00 02003 IEEE 1821 . w(0-IOOQ). Note that. segment insertion are syntactically correct programs. p . the formulae for calculating the impedance are: (a) Z. In our . (3) until a valid individual is generated.M ) and k is the total number of parameters to be optimized. 2. respectively. F. M = iil Thus a new individual. which contains two p e s . the fitting values of the impedance under all other input frequencies can be computed. ... j . the lower the fitness value. is out of its range of definition. 6 > 1) and CO.

we obtain 100 data points (Z:. F(P$).0 00840)L(0. I:=% The parameter settings ofthe HEMA are as follows: in initialize the parameter 'population P ( I ) = ( P ~ ( I ) . The settings of their optimal values depend upon the property of the specific problem.2 folds of f i .&. P2(t).2Circuit I while (f < MAXCA) do The original circuit used to generate the simulated data is begin shown in Fig. It differs from a simple GA in that the search space of crossover is determined by multiple points (M parents) rather than by only two points used in a painvise crossover. i 3 10 IS 20 T i ollm (b) Fig.20~00. '3.using the 'HEMA. (a) ). Its complex plane impedance plot is shown in Fig.600~O)+CPE(3.. b. .. be 1.0. we observe that. M. of the 20 NnS: 2 Results and Discussions (a) There are 13 runs that the HEMA can find the same circuit model as the original one. h = 8. Pdr)). We list some of them below: Model I : 3. we assume the initial frequency.a=-0. Wj'Z 2 1=1 *. 1822 . end end The essence of the GA lies in the random search to the subspace determined by multiple parents.5. -. The adjustable control parameters in the GA include N . For each : ) data'file.1 Generation of Simulated Data and Parameter Settings of HEMA To test the effectiveness of the HEMA.. : llilN Fnm:= F ( P n m 3 := m a F ( I : if (F(Q) < Fm.b=1. 2(a) which is a typical circuit for the simple randomly select M different individuals P i ( L1-W electron transfer reaction with concentration polarization. 0..5.popsize = 100. . for j := 0 to S do .P.. The fitness values of all those circuits equal to 0. MAXGEP = 5 0 in the GA. generate a new individual Qi := calculate F(Qj). := Q.&3 produce M random coefficients (Yj ( i: I-W.).000061 )C(0. Suppose the fitness function is F(x). begin CI420. All the experiments are performed on a Pentium Ill PC (IGHz) and programmed by C language. 2 (b).. and generate the simulated data based on them.000420))) Model 2: +R(4. [ N is the population size) N=50. twenty independent runs are conducted by . By calculating the values of the electrochemical impedance under each frequency f.MAXGA=1000. Not only the structure of the circuit but also the component parameters are exactly consistent with Circuit I. the GEP.p.600000)+((R(5. (il-99).000773)C(0.0IHz and let f. is 0. 2 Simulated Circuit I (a) and its complex plane impedance plot (b) From the experimental results. from PO).M=8.0. F(P2).927744. a. Moreover more than one point (S offspring) are produced from the subspace and the best one is chosen to replace the worst individual in the original parameter population. calculate the fitness of the population F(P(r)) = (F(P. .356660)C(0. end F(Q) := min ~ ( 8 . r:=r+1.82431I ) a (R(4. Then the structure of the GA can be described as follows: Procedure GA begin Z which are used to set up'thr. To be specific.600000)CPE~320CO00. we design two relatively complex circuits (including the parameter values of components) with distinct complex plane impedance plots by ourselves.3 then P.000420)+R(5. S.input data file.S=20. MAXGA. )CPE(43.600000)-C(0. .500000))-C(0.

2 3 4 5 6 Z /ohm 2 -0. 4 1 .00.5 0-1 . it demonstrates that the genetic algorithm used to do parameter optimization is stable and effective.0039298495.71lFj U966nI. 4(b) illustrates its complex plane impedance plot. 3. in most runs. II . . of the 20 runs.Fig. being the maximum 0. . from the fact that those parameter values are exactly the same as the original circuit.0 - 1.3 Circuit I1 The original circuit used to generate the simulated data is shown in Fig.5- L- - 1.I) 2.the minimum 000000MN)2. C(4. 3 The evolving curves of Model I-Model 5 for Circuit I (c) There are another 4 runs that the HEMA can find such models that have slight difference with the original circuit i n the structure but have a small fitness value. I 2 1 ?I Generation Our experimental results show that as for this circuit. . . -0. there are only one run that the HEMA can find the model that has the exactly same structure as the 1823 .0-0. the computer can discover the suitable circuit structure automatically as well as optimize the component parameters simultaneously according to the input data of electrochemical impedance. as for Circuit I.5 1. I n addition. In other words. . the HEMA can find the circuit models whose structure and. In summary. 4(a) and Fig. 4 Simulated Circuit I1 (a) and its complex plane impedance plot (b) I .64 (b) Fig.5- ? $ 0. by running the HEMA.pararneters both exactly coincide with the original circuit. .

442W0.I80991)))-(R(2.6 69721)L(0.95353 We depict the evolving curves of those six models above 0.000005)))) 331) 3 (R(1. of the 20 ruis there are 17 runs that the HEMA finds another kind of circuit structure shown in Fig. .O002l8)C(O. 5(b).702 793)L(O.2258 18)L(0. we surmise that this +R(2.000207)L(0.000005)-((R(6.56591 1)L(0.OOOM)5)-(R(2.411747) 3 (R(2.825903) 3 (R(2.800000)+((R(6.0.0.458685)L(0.original circuit and whose parameters are almost identical with the original one.864127))))) Model 9 Z'lohm (b) Fig. +R(? XO0~K)0r-Ct01~000051-K12 9997061+Rth 001177rLtO BM127lCPFt6 00027 I .8952 19)C(O.000995) 3 (R(2.000005)) +(R(1.402 +L(O.999706)-C(0.00003 I)L(0.466461 IR(83.001178)+L(O.800000)+(((R(0.096000)))) F = 0.01178)L(0.999705)-C(O.487394.577338)CPE(83. But the -(R(2.000318)CPE(78.999705~C(O. the HEMA finds the models (R(2.0005)))) fitness values of those two models are both minor.8 been realized by people yet.OM)OO5)CPE(53.742320)C (0.800000)+(C(O.000000)L(O.999706)))) M o _.799999)+((R(3.O 000100rClO 000015rLtO 657127 )CPE(7.864127))-R(2.864127)) having different structures with the previous two.O00005)))) M d e l 11. 800000~-+-+R(5. From Fig.000000oMK) Most surprisingly.6166l3)R(12.683 136)+(R(6.47 1400) 704573.000005)C(0.864127)R(2.0.5659 11)+L(0.348435.597639)R(S5. Xa).800000)-+-R(6. 47063.. Below we list some of them: Model 7: CISuF) R 2 811) ( O------l R(2 999706Q) 0 .0. Its complex plane impedance plot is shown in Fig.800000)+((U0.999706)-C(0.224784)CPE(47. Although the specific representations of those 1 models are not completely same. 183 153 for Circuit 11 in Fig.000000)-U0.435266))-(R(2.413373)R(41. Model I O - i +RO.800000)+(C(0.692722)R(98.001175) +L(0.0.0000000000 and 0.953301)C(0.999706) -(R(6.OOO323)CPE(39.000005)CPE(lI .999706)C~O a new equivalent circuit for Circuit II which has not is . with 0.O960001CPE(7.000001 )C(O.O00005)R(I.5 - 1 Simulated curve Fining data A 76)R(83.864130)) 1824 . they all can be 7 simplified into the circuit structure shown in Fig. Model 6 +R(I . 102541)R(6. 5 The circuit that occurs most frequently when evolving Circuit II (a) and its complex plane impedance plot (b) From the case that this kind of model turns up so frequently and its fitness is almost 0.O00005~R( 0.644502.0.618154)C( 3 (R(2.778953)L(0.769643)UO.0.799999)+-I R(3.000M)I )-C(0. 6.0000000001 respectively. 954) In the remaining two runs.255279)C(0.43526~R(2. (a) 1. Its fitness value is 0.0. The model is: +R(5.780889)L(0. k 4 R.001177)+L(0.282573. 5(a) and their parameters only have the difference of mantissa with this circuit. we observe that this circuit can fit the simulated data very well and its fitness value is very close to 0. 5(b).2 1 I)CPE( 19. 52)C(O.864130)R(3 1.0.891787)L(0.001175) 0.518849.

H. ' [IOIM. . D. Genetic Programming II: Automatic Discovery of Reusable Programs. (3) The result of parameter optimization is stable and effective. 31-44. 20. I . Bennett 111. and A. Introduction' to Kinetics of Electrode Processes (Third Edition). In most runs. Cambridge.the efticacy of the HEMA in larger circuits which contain more components and parameters in the future. Koza. Genetic Programming: On the Programming of Computers by Means of Natural Selection. 1996. 60133010) and the Special Funds for Major State Basic Research Projects of China (No. some preliminary work of evolving Chemical Circuits by using GEP. [9] C. . Cha. R. The authors wish to thank the anonymous referees for their helpful suggestions for this paper.24. only if the structure of circuit eventually found is identical. 1994. Journal of Electroanalytical Chemistry. F.being optimized are always consistent. R. 6 The evolving curves of Model 6-Model I I for Circuit I I [ I ] C. We need to further test . Genetic Programming Ill: Darwinian Invention and Problem Solving. MA: MIT Press. 1825 . But sometimes it also finds some new structure that has not been recognized by people yet. [7] I. [ 5 ] J. MA: MIT Press. 1986. The whole modeling process needs not the manual intervention.. Macdoald.131. ~~~ -. A. Gene Expression Programming: A New Adaptive Algorithm for Solving Problems. Cambridge. September 10.0 . [6] I. . Impedance Spectroscopy: Old Problems and New Developments.pp. Keane. Meanwhile we will conduct some similar expenm'ents by using standard GP and compare the results with those of this paper. Lehnen. it has some advantages: 1 I) The whole modeline nrccess is done automaticalh. Boukamp. 2001. 1483-1492. Once the electrochemical impedance data are provided. ' Acknowledgements This work was supported by National Natural Science Foundation of China (No. Compared with most available methods. The Applicability and Power of Complex Nonlinear Least Squares for the Analysis of Impedance and Admittance Data. The user himself can control the structure types and the complexity of the circuits flexibly by defining the sets of functions and terminals and the length of tail of a GEP gene. Solid State lonics. [4] J. 4 Conclusions and Future Work The hybrid evolutionary modeling algorithm (HEMA) based on the combination of Gene Expression Programming (GEP) and genetic algorithm (CA) proposed in this paper i s a new evolutionary approach to build the equivalent circuit model for electrochemical impedance. 1992. . Bejing: Science Press. [8] C. Andre. An Introduction to Genetic Algorithm. This paper is. ~ . A. agreement with the original circuit. CA: Morgan Kaufmann Publishers. 2001. Ferreira. Complex Systems. Koza. ( 2 ) The models have great diversity. Schoonman. Mitchell. San Francisco. Electrochimica Acta. invited tutorial of the 6th online World Conference' on Soft Computing in Industrial Applications. 2002. 13(2). MA: MIT Press. Macdoald. the computer can search suitable circuit structures as well as optimize the component parameters simultaneously by itself. the component parameters. Koza. 2002CB211800). S . [3] J. and M. 1999. 77-95. 1982. pp. the HEMA can find the models which are in . 35. Ferreira. J. As for different runs. by running the HEMA. Gene expression programming in problem solving. P. R. Cambridge. A Nonlinear Least Squares Fit Procedure for Analysis of I~~~~~~~~~ Data of Electrochemical Systems. pp. pp. 1990. 87-129. [2] B. Model 8 VI e -10 I 11 References 21 31 41 Generation Fig. R. R.

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An Evolutionary Approach for Modeling the Equivalent Circuit for electrochemical impedance spectroscopy

An Evolutionary Approach for Modeling the Equivalent Circuit for electrochemical impedance spectroscopy

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