CN105137362A - Nondestructive online detection and fault diagnosis method for stack - Google Patents
Nondestructive online detection and fault diagnosis method for stack Download PDFInfo
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- CN105137362A CN105137362A CN201510676896.XA CN201510676896A CN105137362A CN 105137362 A CN105137362 A CN 105137362A CN 201510676896 A CN201510676896 A CN 201510676896A CN 105137362 A CN105137362 A CN 105137362A
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Abstract
The invention discloses a nondestructive online detection and fault diagnosis method for a stack, which belongs to the technical field of solid oxide fuel cells and electrolytic cell stacks. An EIS (Electrochemical Impedance Spectroscopy) method is adopted to acquire impedance spectroscopy data; ADIS is used for analyzing the impedance spectroscopy data and the number of characteristic peaks and corresponding frequency ranges are determined initially; DRT is used for analyzing the impedance spectroscopy data and regularization factors are selected; the number of characteristic peaks and a frequency range in a relaxation time distribution curve are acquired; an alternative equivalent circuit is built; a correct equivalent circuit is selected, a fitting initial value is determined, and a quantitative analysis result is acquired; DRT analysis results in different operation conditions are acquired, the influence factor of each characteristic peak is compared, a home electrochemical process of each DRT characteristic peak is found out, and a stack fault diagnosis comparison table is obtained; and a repletion unit which has poor performance in the case of test or gets performance speed attenuation in the case of operation is subjected to fault reason analysis. The stack experiment efficiency is greatly improved, and the operation cost is reduced.
Description
Technical field
The invention belongs to Solid Oxide Fuel Cell and electrolytic cell heap technical field, particularly a kind of lossless audio coding of pile and method for diagnosing faults.
Background technology
The chemical energy of fuel is electric energy by electrochemical reaction by Solid Oxide Fuel Cell (SolidOxideFuelCells, SOFC).And electrolytic tank of solid oxide (SolidOxideElectrolyticCells, SOEC) is the inverse operation of SOFC in theory, additional electric energy is namely utilized to be hydrogen and oxygen by raw water electrolysis.For improving the generated energy of SOFC or the hydrogen production rate of SOEC, can by the repetitive of multiple SOFC/SOEC superposition composition pile.
Pile service condition harshness (high temperature, high humidity), relate to parts, material is numerous, usually occur that each piece performance is inconsistent in experiment test and operation, the performance of certain a slice or several cell pieces is weak or lack and affect the situation that performance piled by whole electrolytic cell.In addition, in actual motion, occur interruption of service unavoidably, break down as pre-heating system and have a power failure and electrolytic cell all may be caused to pile fast cooling, constant current constant voltage source is run under breaking down and electrolytic cell may being caused to pile up too high voltages.Now conventional pile on-line testing method is as constant current/constant voltage curve method, and I-V curve method cannot provide more Electrochemistry Information except apparent electrolysis performance, is difficult to diagnose the reason of fault and impact and distinguish.Method for diagnosing faults at present for electrolytic cell heap is generally carry out destructive disassembling, and post analysis finds problem place by experiment.But thisly destructively disassemble that post analysis right and wrong are online, ex situ, be irreversible on mated condition of assembly each in pile and the impact of parameter before and after disassembling, be also usually difficult to after even disassembling find out failure cause.Therefore, develop a kind of harmless online pile detection means efficiently for performance evaluation and fault diagnosis very necessary.
Electrochemical impedance spectral method (EIS) is that a kind of ac current signal that adopts carries out disturbance to electrochemical system to be measured, measures the voltage signal of its feedback, and is familiar with electrochemical system impedance behavior to be measured by the response relation analyzing ac signal.EIS method is widely used in the cell of SOFC and SOEC and the research of associated materials, owing to resulting impedance further can be distinguished and be separated, is considered to the powerful that battery and material property evaluation and the reason of decay are analyzed.But the composition of material, structure, interfacial property and transmittance process etc. are mainly paid close attention in this kind of research.To be familiar with and to optimize electrolysis performance no doubt very important from mechanism, but the commercialization of SOFC and SOEC technology will be realized, also need to study battery pile and modular battery heap.Consider that battery pile not only relate to multiple material, multiple parts, structure is relative complex also.Meanwhile, because cell piece area increases, reacting gas and the uneven diffusion causing relaxation phase of distribution of current, also make the reliability of surveyed EIS greatly reduce, and analyzes difficulty and increase.Therefore, the report measurement of EIS and analytical approach being applied to battery pile is considerably less.
The present invention proposes a kind of lossless audio coding and method for diagnosing faults of pile, adopts electrochemical impedance spectral method (EIS) as means of testing; Impedance spectrum discriminant analysis (ADIS), relaxation time distribution (DRT), equivalent circuit method (ECM) organically combine the qualitative and quantitative analysis realizing each electrochemical process in pile as analysis means; By the electrochemical process set up and the relational implementation performance difference of DRT characteristic peak and the online Nondestructive of failure cause; Greatly can improve the conventional efficient of pile, reduce operating cost.
Summary of the invention
The object of the invention is to the lossless audio coding and the method for diagnosing faults that propose a kind of pile, it is characterized in that, comprise the steps:
1) by impedance spectrum testing tool access pile, adopt electrochemical impedance spectral method (EIS) as means of testing, obtain the impedance spectrum data of unit in pile;
2) impedance spectrum discriminant analysis (ADIS) is utilized to step 1) the impedance spectrum data analysis that obtains, tentatively determine the quantity of characteristic peak and corresponding frequency range;
3) utilize relaxation time distribution (DRT) to impedance spectrum data analysis, quantity and the corresponding frequency range at contrast characteristic peak select regularization factors L, obtain characteristic peak quantity and the frequency range of relaxation time distribution curve;
4) the characteristic peak quantity after analyzing according to DRT and frequency range set up alternative equivalent electrical circuit; Characteristic peak crest frequency after the characteristic frequency of contrast equivalent electrical circuit unit block and DRT analyze, selects correct equivalent electrical circuit and determines matching initial value, obtaining quantitative analysis results;
5) step 1 is repeated) to step 4), obtain the DRT analysis result under different operating condition; The influence factor contrasting each characteristic peak finds out the ownership electrochemical process of DRT characteristic peak, obtains the pile fault diagnosis table of comparisons;
6) utilize step 5) the pile fault diagnosis table of comparisons that obtains, to poor-performing in test or repetitive that the very fast decay of performance occurs in running carry out failure reason analysis, find out performance deficiencies reason and failure problems assembly.
Described DRT analyzes required key parameter and obtains based on ADIS analysis result.
The selection of the foundation of described equivalent electrical circuit, screening and matching initial value is the corresponding relation based on characteristic peaks in the time constant of equivalent electrical circuit unit and relaxation time distribution curve.
The described pile fault diagnosis table of comparisons obtains according to the corresponding relation of operating conditions and DRT analysis result.
The invention has the beneficial effects as follows that the method for diagnosing faults for current electrolysis Chi Dui need carry out destructive disassembling, and after disassembling, carry out the problem that non-online, ex situ analyzes, propose a kind of lossless audio coding and method for diagnosing faults of pile; Adopt electrochemical impedance spectral method (EIS) as means of testing; Impedance spectrum discriminant analysis (ADIS), relaxation time distribution (DRT), equivalent circuit method (ECM) organically combine the qualitative and quantitative analysis realizing each electrochemical process in pile as analysis means; The online Nondestructive of performance difference and failure cause is realized by the corresponding relation setting up electrochemical process and DRT characteristic peak; Greatly can improve the conventional efficient of pile, reduce operating cost.
Accompanying drawing explanation
Fig. 1 is a kind of lossless audio coding and method for diagnosing faults process flow diagram of pile.
Fig. 2 is ADIS analysis result figure.
Fig. 3 is DRT analysis result figure.
Fig. 4 is DRT analysis result screening equivalent electrical circuit EC-1 schematic diagram.
Fig. 5 is DRT analysis result screening equivalent electrical circuit EC-2 schematic diagram.
Fig. 6 is the I-V curve map of four batteries in pile.
Fig. 7 is ohmage and the polarization impedance comparison diagram of Cell-2 and Cell-3.
Fig. 8 is Cell-2 and Cell-3DRT result schematic diagram under SOFC pattern.
Fig. 9 is the impedance of Cell-2 and Cell-3 and the variation relation curve map of temperature under SOFC pattern.
Figure 10 is Nyquist and the DRT schematic diagram before and after accident.
Embodiment
The present invention proposes a kind of lossless audio coding and method for diagnosing faults of pile, elaborates to the present invention below in conjunction with the drawings and specific embodiments.
Figure 1 shows that a kind of lossless audio coding and method for diagnosing faults process flow diagram of pile, comprise the steps:
1) by impedance spectrum testing tool access pile, adopt electrochemical impedance spectral method (EIS) as means of testing, obtain the impedance spectrum data of unit in pile;
2) impedance spectrum discriminant analysis (ADIS) is utilized to step 1) the impedance spectrum data analysis that obtains, tentatively determine the quantity of characteristic peak and corresponding frequency range;
3) utilize relaxation time distribution (DRT) to impedance spectrum data analysis, quantity and the corresponding frequency range at contrast characteristic peak select regularization factors L, obtain characteristic peak quantity and the frequency range of relaxation time distribution curve;
4) the characteristic peak quantity after analyzing according to DRT and frequency range set up alternative equivalent electrical circuit; Characteristic peak crest frequency after the characteristic frequency of contrast equivalent electrical circuit unit block and DRT analyze, selects correct equivalent electrical circuit and determines matching initial value, obtaining quantitative analysis results;
5) step 1 is repeated) to step 4), obtain the DRT analysis result under different operating condition; The influence factor contrasting each characteristic peak finds out the ownership electrochemical process of DRT characteristic peak, obtains the pile fault diagnosis table of comparisons;
6) utilize step 5) the pile fault diagnosis table of comparisons that obtains, to poor-performing in test or repetitive that the very fast decay of performance occurs in running carry out failure reason analysis, find out performance deficiencies reason and failure problems assembly.
Wherein, the required key parameter of described DRT analysis obtains based on ADIS analysis result.
Wherein, the selection of the foundation of described equivalent electrical circuit, screening and matching initial value is the corresponding relation based on characteristic peaks in the time constant of equivalent electrical circuit unit and relaxation time distribution curve.
Wherein, the described pile fault diagnosis table of comparisons obtains according to the corresponding relation of operating conditions and DRT analysis result.
At 700 DEG C, SOFC pattern, the gas composition of hydrogen electrode side is 100%H
2time, the EIS under different oxygen electrode atmosphere of test pile; Implement ADIS to analyze, result as shown in Figure 2; The regularization factors being used for DRT analysis is selected in resistance difference change in contrast Fig. 2, and its value is 350, and gained DRT analysis result as shown in Figure 3, has distinguished at least four electrochemical process in Fig. 3: be referred to as P1 by low frequency tremendously high frequency, P2, P3 and P4; Utilize DRT analysis result screen equivalent electrical circuit EC-1 (as shown in Figure 4) and EC-2 (as shown in Figure 5) and select suitable matching initial value, complete quantitative test;
DRT analyzes and relaxation time distribution corresponding to impedance spectrum gives, and the extreme value place i.e. characteristic time of a corresponding electrochemical process of each characteristic peak, be called relaxation time τ, computing formula is:
Wherein, f is relaxation frequency.
ECM by setting up equivalent electrical circuit, with the impedance behavior of equivalent-circuit component analog electrical chemical system, the wherein every corresponding electrochemical process of group/equivalence element.Therefore, the characteristic time of the equivalence element in a rational ECM fitting result should be consistent with the relaxation time in DRT.
To RQ element, time constant T
rQcan be expressed as:
Wherein, R is resistance; Q is constant phase angle element value; n
qfor dimensionless group.
The time constant T of Warburg element
wbe shown below:
Wherein, Z
wfor the impedance of Warburg element; R
wfor the resistance of Warburg element; I is imaginary symbols; ω is angular frequency.
The time constant T of Gerischer element
gmeet:
Wherein, Z
gfor the impedance of Gerischer element; I is imaginary symbols; ω is angular frequency; R
gfor the resistance of Gerischer element.
In the relaxation time obtained by DRT method and ECM fitting result, the time constant list of each equivalence element is as shown in table 1;
The table relaxation time of 1DRT and the time constant contrast table of ECM
In table 1, wherein relaxation time t
1: t
4p1 ~ P4 in corresponding DRT figure.Visible, when adopting EC-1 to carry out matching, the time constant of RQ and the Warburg element of low-frequency range and relaxation time t
1and t
2inconsistent, error of fitting is 6.3%.After Warburg element is replaced with RQ element, t
2situation improves, but t
1gap still comparatively large, error of fitting is 5.9%.Then, adopt the matching again of new initial value, obtain desirable fitting result, error of fitting is only 1.0%, each time constant and relaxation time one_to_one corresponding.The fitting result of the corresponding EC-2 obtained is as shown in table 2;
Table 2 Equivalent Circuit Fitting result parameter
The corresponding relation of being tested electrochemical process and the DRT characteristic peak determined by variation of operating parameters is as shown in table 3; Above-mentioned analysis result is utilized to carry out pile diagnosis.
The table 3DRT characteristic peak table of comparisons
The analysis of causes of (a) problem sheet
Figure 6 shows that (700 DEG C, SOFC pattern, hydrogen electrode gas composition is 80%H for the I-V curve of four batteries in pile
2, 20%H
2o), be the poorest problem sheet of performance in four battery pile by the known Cell-2 of IV curve of Fig. 6, existing trial utilizes said method to find out performance difference reason.
By Cell-2 and Cell-3 at 700 DEG C, hydrogen electrode atmosphere is 100% hydrogen; 700 DEG C, hydrogen electrode water vapour content is 20%; 750 DEG C, hydrogen electrode water vapour content be 20% 3 kind of condition under ohmage and polarization impedance compare, as shown in Figure 7; Visible, under three kinds of conditions, the equal no significant difference of polarization impedance of Cell-2 and Cell-3, resistance difference is mainly ohmage part.
For proving this conclusion further, by Cell-2 and Cell-3 under SOFC pattern, when the change of hydrogen electrode atmosphere, the change of oxygen electrode atmosphere and temperature variation time DRT result compare, be illustrated in figure 8 the DRT result of Cell-2 and Cell-3 under the change of (a) hydrogen electrode side atmosphere, the change of (b) oxygen electrode side atmosphere, (c) temperature variation under SOFC pattern; Because the size of polarization impedance is relevant with the peak area of DRT characteristic peak.Can intuitively find out, the impedance magnitude of Cell-2 with Cell-3 under each operating conditions and variation relation all consistent.Determine that the difference of Cell-2 and Cell-3 is not polarization impedance part thus.
Ohmage is the main source of Cell-2 and Cell-3 performance difference, and the ohmage in battery pile mainly comprises the Ohmage of cell piece and the contact resistance in heap.Under the condition that contact is good, the resistance of contact resistance varies with temperature similar to the variation relation of temperature to contact material used itself.Owing to adopting same material, composition and preparation technology, when contacting good, the ohmage of Cell-2 with Cell-3 should be consistent with the variation relation of temperature.As shown in Figure 9, the ohmage of Cell-2 with Cell-3 is substantially identical with the variation relation parameter of temperature, judges that the performance difference of two panels cell piece is mainly due to the impact of contact resistance thus.
(b) accident diagnosis
Due to misoperation in experimentation, cause battery pile under hydrogen electrode liquid water content is the condition of 0% in SOEC mode operation a period of time, result causes electrolytic cell to pile performance rapid decay.Diagnostic method of the present invention is utilized to analyze to problem sheet Cell-2 and normal sheet Cell-3 the main cause that the accident of finding out causes electrical property to decline.
Table 4 is problem sheet Cell-2 and the normal ohmage of sheet Cell-3 and the change list of polarization impedance before and after accident.
Impedance contrast before and after table 4Cell-2 and Cell-3 accident
Figure 10 is that (a) Nyquist before and after accident schemes, (b) DRT schemes (700 DEG C, SOFC pattern, hydrogen electrode is 100%H2, and oxygen electrode is air).
First, normal sheet Cell-3 is analyzed.Before and after accident, the ohmage of Cell-3 is almost constant, and polarization impedance sharply increases by 42%.Corresponding DRT analysis result as shown in Figure 10 (b), the characteristic peak P4 that the charge transfer at the increase part main hydrogen electrode three phase boundary place of polarization impedance is relevant with the ion conduction processes in YSZ skeleton.Consider under experimental conditions, because hydrogen electrode does not have the water vapor of supply electrolytic reaction, Faradaic current may change the microstructure at three phase boundary place, causes performance degradation.
Secondly, consider a problem sheet Cell-2, and its decling phase is more more serious than Cell-3, and ohmic part increases 65%, and polarized portions adds 145%.This is that electrolysis adopts constant current mode, and because Cell-2 performance is the poorest, in process, this cell piece has the highest dividing potential drop, therefore there occurs more serious decay.
To sum up, the interruption of service carrying out constant-current electrolysis under dry hydrogen electrode atmosphere causes pile apparent property to decay, method for diagnosing faults of the present invention is utilized to recognize: on the one hand, decay mainly occurs in polarization impedance part, specifically, this accident destroys the electrode microstructure at the three phase boundary place of hydrogen electrode thus causes performance sharply to decline; On the other hand, the dividing potential drop of the problem sheet of the poor-performing in battery pile is higher, and when adding all too high decomposition voltages to pile, problem sheet institute is influenced larger.
The present invention proposes a kind of lossless audio coding and method for diagnosing faults of pile; Adopt electrochemical impedance spectral method (EIS) as means of testing; Impedance spectrum discriminant analysis (ADIS), relaxation time distribution (DRT), equivalent circuit method (ECM) organically combine the qualitative and quantitative analysis realizing each electrochemical process in pile as analysis means; Realize not lowering the temperature and carrying out Nondestructive to the performance difference between electric pile unit and pile failure cause under not tearing heap situation open by the corresponding relation setting up electrochemical process and DRT characteristic peak, not only avoid cooling, tear change and destroying infection diagnostic result that the operation such as heap causes electric pile structure and surface open, carry out online failure reason analysis simultaneously and also contribute to Optimal Experimental operation, the possibility reducing pile decay and lost efficacy, even complete the eliminating of fault, thus greatly improve the conventional efficient of pile, reduce operating cost.
The above; be only the present invention's preferably embodiment, but protection scope of the present invention is not limited thereto, is anyly familiar with those skilled in the art in the technical scope that the present invention discloses; the change that can expect easily or replacement, all should be encompassed within protection scope of the present invention.Therefore, protection scope of the present invention should be as the criterion with the protection domain of claim.
Claims (4)
1. the lossless audio coding of pile and a method for diagnosing faults, is characterized in that, comprise the steps:
1) by impedance spectrum testing tool access pile, adopt electrochemical impedance spectral method (EIS) as means of testing, obtain the impedance spectrum data of unit in pile;
2) impedance spectrum discriminant analysis (ADIS) is utilized to step 1) the impedance spectrum data analysis that obtains, tentatively determine the quantity of characteristic peak and corresponding frequency range;
3) utilize relaxation time distribution (DRT) to impedance spectrum data analysis, quantity and the corresponding frequency range at contrast characteristic peak select regularization factors L, obtain characteristic peak quantity and the frequency range of relaxation time distribution curve;
4) the characteristic peak quantity after analyzing according to DRT and frequency range set up alternative equivalent electrical circuit; Characteristic peak crest frequency after the characteristic frequency of contrast equivalent electrical circuit unit block and DRT analyze, selects correct equivalent electrical circuit and determines matching initial value, obtaining quantitative analysis results;
5) step 1 is repeated) to step 4), obtain the DRT analysis result under different operating condition; The influence factor contrasting each characteristic peak finds out the ownership electrochemical process of DRT characteristic peak, obtains the pile fault diagnosis table of comparisons;
6) utilize step 5) the pile fault diagnosis table of comparisons that obtains, to poor-performing in test or repetitive that the very fast decay of performance occurs in running carry out failure reason analysis, find out performance deficiencies reason and failure problems assembly.
2. a kind of lossless audio coding of pile and method for diagnosing faults according to claim 1, it is characterized in that, described DRT analyzes required key parameter and obtains based on ADIS analysis result.
3. a kind of lossless audio coding of pile and method for diagnosing faults according to claim 1, it is characterized in that, the selection of the foundation of described equivalent electrical circuit, screening and matching initial value is the corresponding relation based on characteristic peaks in the time constant of equivalent electrical circuit unit and relaxation time distribution curve.
4. a kind of lossless audio coding of pile and method for diagnosing faults according to claim 1, it is characterized in that, the described pile fault diagnosis table of comparisons obtains according to the corresponding relation of operating conditions and DRT analysis result.
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