CN114361535B - Fuel cell hydrogen permeation quantity assessment method based on electrochemical impedance spectrum - Google Patents
Fuel cell hydrogen permeation quantity assessment method based on electrochemical impedance spectrum Download PDFInfo
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- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention relates to a fuel cell hydrogen permeation quantity assessment method based on electrochemical impedance spectrum, the method comprises the following steps: s1, determining the operation condition of impedance test; s2 dividing all single cells in the fuel cell stack into a plurality of groups according to the sequence; s3, obtaining electrochemical impedance spectrums of the battery packs through impedance tests; s4, fitting impedance data by using the equivalent circuit model to obtain the resistance value of a specific element in the equivalent circuit model; s5, comparing the resistance values of specific elements in each battery pack and judging the position of the fuel cell stack where the hydrogen permeation quantity is maximum; s6 establishing a corresponding relation between the hydrogen permeation quantity and the resistance value of each battery pack through a voltage transformation test; and S7, in the aging process of the fuel cell stack, judging the change condition of the hydrogen permeation quantity based on the change of the resistance value of each cell group, and estimating the hydrogen permeation quantity of each cell group according to the established corresponding relation between the resistance value and the hydrogen permeation quantity. Compared with the prior art, the invention has the advantages of low cost, high test speed, high accuracy and the like.
Description
Technical Field
The invention relates to the technical field of proton exchange membrane fuel cells, in particular to a fuel cell hydrogen permeation quantity assessment method based on electrochemical impedance spectroscopy.
Background
The proton exchange membrane fuel cell automobile has become one of the important development directions of the next generation electric automobile by virtue of the advantages of low working temperature, high conversion efficiency, environmental friendliness, flexible assembly and the like, but at present, the fuel cell has a plurality of problems, wherein the service life problem is one of key factors restricting the commercialization process of the fuel cell automobile, the primary problem faced by the current service life optimization of the fuel cell is how to quantify the service life attenuation of the fuel cell, and in recent years, the hydrogen permeation quantity has become one of new promotion indexes for representing the aging state of the fuel cell, and the hydrogen introduced by the anode of the fuel cell can inevitably permeate to the cathode through the electrolyte membrane when the fuel cell works due to the certain pore characteristics of the proton exchange membrane. The existence of hydrogen permeation in the fuel cell not only reduces the working efficiency of the cell, but also can cause irreversible damage to the catalytic layer and the membrane structure, and along with the gradual aging of the proton exchange membrane, the hydrogen permeation quantity in the fuel cell is continuously increased, on the other hand, because the initial performance of the fuel cell after leaving the factory has certain difference, the use environment of each single cell in the electric pile is not completely the same, the inconsistency of the electric pile hydrogen permeation can be gradually amplified along with the time, and therefore, the effective measurement of the electric pile hydrogen permeation distribution has important significance for the life prediction, fault diagnosis and consistency assessment of the fuel cell.
One of the common methods for measuring hydrogen permeation of fuel cells is a microanalysis method, which is based on the principle that a trace substance analyzer is used to measure the volume fraction of trace hydrogen in the cathode exhaust gas of the fuel cells, and then the hydrogen permeation value is obtained through calculation.
Another common method is voltammetry, which is a principle that a certain form of voltage excitation is applied to a fuel cell, and then the hydrogen permeation flow value inside the cell is obtained by analyzing a response current signal, and is only suitable for hydrogen permeation measurement of single cells, if a scanning voltage is applied between two poles of a galvanic pile, partial pressure of each single cell inside the cell will change irregularly, uncontrollable voltage excitation cannot achieve a corresponding test purpose, if the voltammetry is used for measuring each single cell in the galvanic pile one by one, periodic galvanic pile hydrogen permeation detection will consume a large amount of time, and meanwhile, the corresponding test has higher requirements on the number of channels of hardware, so that development of a galvanic pile hydrogen permeation measurement method with low cost and high test speed is necessary to overcome the limitations of the prior art.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provide a fuel cell hydrogen permeation quantity assessment method based on electrochemical impedance spectroscopy.
The aim of the invention can be achieved by the following technical scheme:
a fuel cell hydrogen permeation quantity evaluation method based on electrochemical impedance spectroscopy, comprising the following steps:
s1, determining the operation condition of impedance test;
s2, dividing all single cells in the fuel cell stack into a plurality of groups according to the sequence, wherein each n single cells form a group of cell groups and correspond to a voltage acquisition channel, and n is more than or equal to 1;
s3, obtaining electrochemical impedance spectrums of the battery packs through impedance tests;
s4, fitting impedance data by using the equivalent circuit model to obtain the resistance value of a specific element in the equivalent circuit model;
s5, comparing the resistance values of specific elements in each battery pack and judging the position of the fuel cell stack where the hydrogen permeation quantity is maximum;
s6, establishing a corresponding relation between the hydrogen permeation quantity and the resistance value of each battery pack through a voltage transformation test;
and S7, in the aging process of the fuel cell stack, judging the change condition of the hydrogen permeation quantity based on the change of the resistance value of each cell group, and estimating the hydrogen permeation quantity of each cell group according to the established corresponding relation between the resistance value and the hydrogen permeation quantity.
In the step S1, the impedance test is performed in a set air intake environment, that is, hydrogen is introduced into the anode side of the fuel cell stack, and inert gas is introduced into the cathode side, where the inert gas is one or a mixture of a plurality of nitrogen, air after oxygen removal, and rare gas.
In the step S1, the operating conditions of the impedance test include an intake pressure, an intake humidity, a fuel cell stack temperature, and ac impedance test parameters, where the intake pressure, the intake humidity, and the fuel cell stack temperature remain constant during the impedance test, and the ac impedance test parameters include a disturbance signal form, an ac amplitude, and a frequency range for impedance measurement.
The step S3 specifically comprises the following steps:
and applying disturbance current with set amplitude and no direct current bias to the fuel cell stack through the controllable current source, simultaneously acquiring disturbance current data and response voltage data of each cell group, and acquiring electrochemical impedance spectrums of the cell groups based on the acquired data.
The equivalent circuit model consists of a first resistor element R 0 Second resistor element R 1 And a constant phase angle element CPE, said second resistance element R 1 In parallel with the CPE, and after having been connected to the CPE, with a constant phase angle 0 In series with a second resistance element R 1 As a specific element, its resistance value is acquired.
In the step S5, the specific method for determining the position with the larger hydrogen permeation amount in the fuel cell stack is as follows:
second resistive element R relative to the remaining battery pack 1 The position of the battery pack with the minimum resistance value is the position with the maximum hydrogen permeation quantity of the fuel cell stack.
The step S6 specifically comprises the following steps:
s61 of changing the intake pressure on the anode side based on the operation condition determined in step S1;
s62, measuring hydrogen permeation quantity of each battery pack under different constant air inlet pressure and corresponding second resistance element R 1 Resistance value;
s63, establishing a second resistance element R for each battery pack 1 A table or a functional relation of the resistance value and different hydrogen permeation amounts.
In the step S62, the hydrogen permeation quantity is measured by a voltammetry or constant current charging method, and the second resistance element R is realized by the steps S2-S4 1 And (5) measuring the resistance.
The step S7 specifically comprises the following steps:
s71, during the aging process of the fuel cell stack, measuring each cell group according to the steps S2-S4 under the operation condition of the step S1Second resistance element R 1 Resistance value;
s72, if the second resistance element R of a certain group of batteries is measured 1 The resistance value is reduced relative to the previous time point, and the hydrogen permeation quantity of the battery pack is judged to be increased;
s73 respectively according to the established second resistance element R 1 Relation table of resistance value and hydrogen permeation quantity or second resistance element R 1 And estimating the hydrogen permeation quantity of the battery pack according to a functional relation between the resistance value and the hydrogen permeation quantity.
In the step S73, if the second resistor R of each battery is established 1 A relation table of the resistance value and the hydrogen permeation quantity, and a second resistance element R of each battery pack is measured 1 The resistance value is used as an index, and the corresponding hydrogen permeation quantity is searched out from the established relation table by utilizing an interpolation table lookup method, namely, the estimated hydrogen permeation quantity value of each battery pack at the time point is obtained; if the second resistance element R of each battery pack is established 1 The second resistance element R of each battery pack is measured according to the functional relation between the resistance value and the hydrogen permeation quantity 1 And substituting the resistance value into the established functional relation, and calculating the corresponding hydrogen permeation quantity, namely, the estimated hydrogen permeation quantity value of each battery pack at the time point.
Compared with the prior art, the invention has the following advantages:
1. low cost: the method is based on electrochemical technology to measure hydrogen permeation distribution of the galvanic pile, realizes accurate estimation of hydrogen permeation quantity according to the relation between specific elements and hydrogen permeation quantity in an equivalent circuit model, does not need to rely on expensive high-precision analysis instruments, supports combination detection of a plurality of batteries, and has flexible requirements on the number of data acquisition channels.
2. The test speed is high: the alternating current impedance test in the method takes alternating current as an excitation signal, the test of each battery in the electric pile can be carried out simultaneously, and the test time is not prolonged along with the increase of the number of the battery pieces.
Drawings
FIG. 1 is a schematic general flow chart of the present invention.
Fig. 2 is an exemplary diagram of an equivalent circuit model for impedance data fitting in an embodiment.
Fig. 3 is a diagram showing an example of the resistance values of each battery pack obtained by fitting an equivalent circuit model in the embodiment.
Fig. 4 is a graph showing the correspondence between the resistance value of a single cell and different hydrogen permeation amounts in the embodiment.
Detailed Description
The invention will now be described in detail with reference to the drawings and specific examples.
As shown in fig. 1, the present invention provides a fuel cell hydrogen permeation quantity evaluation method based on electrochemical impedance spectroscopy, which comprises the following steps:
s1, determining the operation condition of impedance test;
s2, dividing all single cells in the fuel cell stack into a plurality of groups according to the sequence, wherein n single cells form a group corresponding to a voltage acquisition channel, and n is more than or equal to 1;
s3, obtaining electrochemical impedance spectrums of the battery packs through impedance tests;
s4, fitting impedance data by using the equivalent circuit model to obtain the resistance value of a specific element in the equivalent circuit model;
s5, comparing the resistance values of specific elements in each battery pack and judging the position with larger hydrogen permeation quantity in the fuel cell stack;
s6, establishing a corresponding relation between the hydrogen permeation quantity and the resistance value of each battery pack through a voltage transformation test;
and S7, in the aging process of the fuel cell stack, judging the change condition of the hydrogen permeation quantity based on the change of the resistance value of each cell group, and estimating the hydrogen permeation quantity of each cell group according to the established corresponding relation between the resistance value and the hydrogen permeation quantity.
In the step S1, the impedance test is performed in a set air inlet environment, namely, hydrogen is introduced into the anode side of the fuel cell stack, and inert gas is introduced into the cathode side, wherein the inert gas adopts one or a mixture of more of nitrogen, air after oxygen is removed and rare gas;
the operating conditions include intake pressure, intake humidity, fuel cell stack temperature, and ac impedance test parameters including disturbance signal form, ac amplitude, and frequency range for impedance measurement, with the intake pressure, intake humidity, fuel cell stack temperature remaining constant during impedance testing.
In step S3, the specific manner of obtaining the electrochemical impedance spectrum of each battery pack through the impedance test is as follows:
and applying disturbance current with set amplitude (the disturbance current has no direct current bias) to the fuel cell stack through the controllable current source, collecting disturbance current data and response voltage data of each cell group, and calculating to obtain the electrochemical impedance spectrum of each cell group based on the collected data.
In step S4, the equivalent circuit model is mainly composed of a resistor R 0 Resistor element R 1 And a constant phase angle element CPE, a resistor element R 1 Parallel to CPE and then connected to R 0 In series with a resistor element R 1 As a specific element, and acquires its resistance value.
In step S5, the specific method for determining the position in the fuel cell stack where the hydrogen permeation amount is large is:
resistance element R relative to the remaining cells 1 The group of cells with the significantly smaller resistance (smallest) is located at the position where the hydrogen permeation amount of the fuel cell stack is larger (largest).
The step S6 specifically comprises the following steps:
s61, changing the inlet pressure of the hydrogen side on the basis of the operation condition of the step S1;
s62, measuring hydrogen permeation quantity and corresponding R of each battery pack under different constant air inlet pressure 1 Resistance, hydrogen permeation quantity is measured by voltammetry or constant current charging method, R 1 The resistance is realized through the steps S2-S4;
s63, building R for each battery pack 1 A table or a functional relation of the resistance value and different hydrogen permeation amounts.
The step S7 specifically includes the following steps:
s71, at a certain time point in the aging process of the fuel cell stack, measuring R of each cell group according to steps S2-S4 under the operation condition of the step S1 1 Resistance value;
s72, if R of a certain group of batteries is measured 1 Resistance value relative to upperWhen the time point is obviously reduced, judging that the hydrogen permeation quantity of the group of batteries is increased;
s73, if each battery group R is established 1 A relation table of resistance and hydrogen permeation quantity, then R of each battery pack is measured 1 The resistance value is used as an index, and the corresponding hydrogen permeation quantity is searched out from the established relation table by utilizing an interpolation table lookup method, namely, the estimated hydrogen permeation quantity value of each battery pack at the time point is obtained; if each battery group R is established 1 The R of each battery pack is measured according to the functional relation between the resistance and the hydrogen permeation quantity 1 And substituting the resistance value into the established functional relation, and calculating the corresponding hydrogen permeation quantity, namely, the estimated hydrogen permeation quantity value of each battery pack at the time point.
Examples
The test object of the embodiment is a proton exchange membrane fuel cell short stack, and the practical application is not limited to this.
With a reaction area of 25cm 2 In the case of a short stack of 10 cells, hydrogen was introduced into the anode, nitrogen was introduced into the cathode, the air inlet pressure was atmospheric pressure, the air inlet humidity was 50%, and the stack temperature was maintained at 60 ℃.
Dividing all single cells in a fuel cell stack into 10 groups according to the sequence, wherein 1 single cell forms a group corresponding to a voltage acquisition channel, applying small-amplitude disturbance current to the fuel cell stack through a controllable current source, simultaneously acquiring disturbance current data and response voltage data of each cell group, and calculating to obtain the electrochemical impedance spectrum of each cell group based on the acquired data.
FIG. 2 is an example diagram of an equivalent circuit model for impedance data fitting, the model consisting essentially of a resistive element R 0 Resistor element R 1 And a constant phase angle element CPE, a resistor element R 1 Parallel to CPE and then connected to R 0 And (3) connecting in series.
FIG. 3 is an exemplary plot of the resistance of each battery obtained by model fitting, R for a first set of cells relative to the remaining cells 1 The resistance is significantly smaller and therefore the first group of cells is the location in the fuel cell stack where the hydrogen permeation amount is greater.
Based on the aforementioned operating conditionsIncreasing the air inlet pressure of the hydrogen side of the fuel cell stack, and measuring the hydrogen permeation quantity and the corresponding R of each cell group under different constant air inlet pressure 1 Resistance value. The hydrogen permeation amount was measured by voltammetry.
Fig. 4 is a diagram showing an example of the correspondence between the resistance value of a single cell and different hydrogen permeation amounts. Taking the measurement result of the first group of cells shown in the figure as an example, at a certain point in time during the aging of the fuel cell stack, if the R of the first group of cells is measured under the condition that the intake air pressure is the same as the atmospheric pressure 1 The resistance value is obviously smaller than the corresponding value of the 0kPa data point in the graph, the hydrogen permeation quantity of the group of batteries is judged to be increased, and the measured R is further judged to be 1 And taking the resistance value as an index, and interpolating to obtain the hydrogen permeation estimated value of the first group of batteries at the time point according to the corresponding relation between the measured resistance value and the hydrogen permeation quantity.
The foregoing description of the embodiments of the invention is not intended to be limiting, but rather should be utilized to limit the scope of the invention.
Claims (7)
1. A fuel cell hydrogen permeation quantity evaluation method based on electrochemical impedance spectroscopy, which is characterized by comprising the following steps:
s1, determining the operation condition of impedance test;
s2, dividing all single cells in the fuel cell stack into a plurality of groups according to the sequence, wherein each n single cells form a group of cell groups and correspond to a voltage acquisition channel, and n is more than or equal to 1;
s3, obtaining electrochemical impedance spectrums of the battery packs through impedance tests;
s4, fitting impedance data by using the equivalent circuit model to obtain the resistance value of a specific element in the equivalent circuit model;
s5, comparing the resistance values of specific elements in each battery pack and judging the position of the fuel cell stack where the hydrogen permeation quantity is maximum;
s6, establishing a corresponding relation between the hydrogen permeation quantity and the resistance value of each battery pack through a voltage transformation test;
s7, in the aging process of the fuel cell stack, judging the change condition of the hydrogen permeation quantity based on the change of the resistance value of each cell group, and estimating the hydrogen permeation quantity of each cell group according to the established corresponding relation between the resistance value and the hydrogen permeation quantity;
in the step S1, the impedance test is performed in a set air inlet environment, namely, hydrogen is introduced into the anode side of the fuel cell stack, and nitrogen is introduced into the cathode side of the fuel cell stack;
the equivalent circuit model consists of a first resistor element R 0 Second resistor element R 1 And a constant phase angle element CPE, said second resistance element R 1 In parallel with the CPE, and after having been connected to the CPE, with a constant phase angle 0 In series with a second resistance element R 1 As a specific element, acquiring a resistance value thereof;
the step S6 specifically comprises the following steps:
s61 of changing the intake pressure on the anode side based on the operation condition determined in step S1;
s62, measuring hydrogen permeation quantity of each battery pack under different constant air inlet pressure and corresponding second resistance element R 1 Resistance value;
s63, establishing a second resistance element R for each battery pack 1 A table or a functional relation of the resistance value and different hydrogen permeation amounts.
2. The method according to claim 1, wherein in the step S1, the operating conditions of the impedance test include an intake pressure, an intake humidity, a fuel cell stack temperature, and an ac impedance test parameter, the intake pressure, the intake humidity, and the fuel cell stack temperature being constant during the impedance test, the ac impedance test parameter including a disturbance signal form, an ac amplitude, and a frequency range for impedance measurement.
3. The method for evaluating hydrogen permeation quantity of fuel cell based on electrochemical impedance spectroscopy according to claim 1, wherein the step S3 specifically comprises:
and applying disturbance current with set amplitude and no direct current bias to the fuel cell stack through the controllable current source, simultaneously acquiring disturbance current data and response voltage data of each cell group, and acquiring electrochemical impedance spectrums of the cell groups based on the acquired data.
4. The method for evaluating hydrogen permeation quantity of fuel cell based on electrochemical impedance spectroscopy according to claim 1, wherein in the step S5, the specific way for determining the position in the fuel cell stack where the hydrogen permeation quantity is large is as follows:
second resistive element R relative to the remaining battery pack 1 The position of the battery pack with the minimum resistance value is the position with the maximum hydrogen permeation quantity of the fuel cell stack.
5. The method for evaluating hydrogen permeation quantity of fuel cell based on electrochemical impedance spectrum according to claim 1, wherein in step S62, hydrogen permeation quantity is measured by voltammetry or constant current charging method, and the second resistance element R is realized by steps S2-S4 1 And (5) measuring the resistance.
6. The method for evaluating hydrogen permeation quantity of fuel cell based on electrochemical impedance spectroscopy according to claim 1, wherein said step S7 specifically comprises the steps of:
s71, during the aging of the fuel cell stack, measuring the second resistance element R of each cell group according to steps S2-S4 under the operation condition of step S1 1 Resistance value;
s72, if the second resistance element R of a certain group of batteries is measured 1 The resistance value is reduced relative to the previous time point, and the hydrogen permeation quantity of the battery pack is judged to be increased;
s73, respectively according to the established second resistance element R 1 Relation table of resistance value and hydrogen permeation quantity or second resistance element R 1 And estimating the hydrogen permeation quantity of the battery pack according to a functional relation between the resistance value and the hydrogen permeation quantity.
7. The method for evaluating hydrogen permeation quantity of fuel cell based on electrochemical impedance spectroscopy according to claim 6, wherein in step S73, if the second resistance of each cell group is establishedElement R 1 A relation table of the resistance value and the hydrogen permeation quantity, and a second resistance element R of each battery pack is measured 1 The resistance value is used as an index, and the corresponding hydrogen permeation quantity is searched out from the established relation table by utilizing an interpolation table lookup method, namely, the estimated hydrogen permeation quantity value of each battery pack at the time point is obtained; if the second resistance element R of each battery pack is established 1 The second resistance element R of each battery pack is measured according to the functional relation between the resistance value and the hydrogen permeation quantity 1 And substituting the resistance value into the established functional relation, and calculating the corresponding hydrogen permeation quantity, namely, the estimated hydrogen permeation quantity value of each battery pack at the time point.
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