CN114373967A - Method for measuring hydrogen permeation quantity of fuel cell stack - Google Patents
Method for measuring hydrogen permeation quantity of fuel cell stack Download PDFInfo
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04298—Processes for controlling fuel cells or fuel cell systems
- H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
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- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04298—Processes for controlling fuel cells or fuel cell systems
- H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
- H01M8/0444—Concentration; Density
- H01M8/04447—Concentration; Density of anode reactants at the inlet or inside the fuel cell
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- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04298—Processes for controlling fuel cells or fuel cell systems
- H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
- H01M8/0444—Concentration; Density
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- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04298—Processes for controlling fuel cells or fuel cell systems
- H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
- H01M8/04537—Electric variables
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Abstract
The invention relates to a method for measuring the hydrogen permeation quantity of a fuel cell stack, which comprises the following steps: s1, introducing hydrogen into the anode side of the fuel cell stack, introducing inert gas into the cathode side, and keeping the pressure of the introduced gas on the two sides and the temperature of the fuel cell stack at constant levels; s2, sequentially charging the fuel cell stack by constant charging currents with different magnitudes; s3, recording the voltage response of the fuel cell stack under each charging current; s4, acquiring a differential curve of voltage response; s5, extracting characteristic point information on the differential curve and a corresponding charging current value; s6, fitting a function model according to the extracted feature point information and the charging current value to obtain parameter values of the function model, and determining equivalent current of hydrogen permeation quantity in each single battery; and S7, obtaining the hydrogen permeation amount in each single battery through conversion. Compared with the prior art, the method has the advantages of accurate test, strong operability and the like.
Description
Technical Field
The invention relates to the technical field of proton exchange membrane fuel cells, in particular to a method for measuring hydrogen permeation quantity of a fuel cell stack.
Background
Compared with other new energy sources, the proton exchange membrane fuel cell has the characteristics of low working temperature, high conversion efficiency, environmental friendliness and simple and flexible assembly, by virtue of the advantages, a fuel cell automobile becomes one of important development directions of next-generation electric automobiles, however, in terms of current practice, the fuel cell still has a plurality of problems, wherein the service life problem is one of key factors for restricting large-scale application and commercialization of the fuel cell, the primary challenge in service life optimization is to quantify the aging state of the fuel cell, in recent years, the hydrogen permeation quantity becomes one of new promotion indexes for evaluating the service life attenuation of the proton exchange membrane fuel cell, and the accurate measurement of the hydrogen permeation distribution of the galvanic pile has important significance for service life prediction, fault diagnosis and consistency evaluation of the fuel cell.
For the quantitative detection of the hydrogen permeation amount, the existing method is a microanalysis method, the basic principle is that the content of hydrogen in the gas at the cathode outlet of the fuel cell is quantitatively detected through a gas chromatograph or a mass spectrometer, so that the hydrogen permeation amount is determined, a detection instrument used in the method is extremely expensive, the corresponding operation flow is complex, complicated sampling and calibration steps are needed, and the popularization and the application cannot be realized.
Another common method is sweep voltammetry, which has the basic principle that voltage excitation in a specific form is applied to a fuel cell, and then a hydrogen permeation flow rate value is indirectly obtained by collecting and analyzing a response current signal.
In the prior art related to galvanic pile hydrogen permeation detection, Chinese patents: a method for detecting the membrane electrode series leakage in the running process of a fuel cell vehicle (CN112414633A), a method for detecting the membrane electrode series leakage of a fuel cell stack (CN111106370A) and a method for quickly detecting the hydrogen and oxygen series gas of the fuel cell stack (CN101697005A) mainly adopt a method for judging the hydrogen permeation size based on voltage change, the qualitative detection method is difficult to accurately reflect the nonlinear change process of the hydrogen permeation amount of the fuel cell in the whole life cycle, the detection result has very limited help on life prediction and failure diagnosis, and no mature technology exists for the quantitative detection of the hydrogen permeation of a plurality of stacks at present.
Chinese patent: the fuel cell stack membrane electrode parameter detection method and the detection device (CN110703102A) provide that current excitation is applied to a stack under the condition of sealing two electrode gas inlets and two electrode gas outlets, and then hydrogen permeation parameters of the stack are obtained by analyzing response voltage signals, but the operation condition causes the flow of cathode gas to be limited, the cell voltage cannot reach a stable state due to continuous permeation and adsorption of reaction gas on the other side, and the accumulation of the reaction gas can seriously influence the electrochemical measurement result, so the method has low feasibility. Therefore, it is necessary to develop a quantitative detection method for hydrogen permeation of a galvanic pile, which has accurate test and strong operability, so as to overcome the limitations of the prior art.
Disclosure of Invention
The present invention is directed to a method for measuring hydrogen permeation rate of a fuel cell stack, which overcomes the above-mentioned drawbacks of the prior art.
The purpose of the invention can be realized by the following technical scheme:
a method for measuring hydrogen permeation quantity of a fuel cell stack, comprising the steps of:
s1, introducing hydrogen into the anode side of the fuel cell stack, introducing inert gas into the cathode side, and keeping the pressure of the introduced gas on the two sides and the temperature of the fuel cell stack at constant levels;
s2, sequentially charging the fuel cell stack by constant charging currents with different magnitudes;
s3, recording the voltage response of the fuel cell stack under each charging current;
s4, acquiring a differential curve of voltage response;
s5, extracting characteristic point information on the differential curve and a corresponding charging current value;
s6, fitting a function model according to the extracted feature point information and the charging current value to obtain parameter values of the function model, and determining equivalent current of hydrogen permeation quantity in each single battery;
and S7, obtaining the hydrogen permeation amount in each single battery through conversion.
In step S1, the inert gas is nitrogen, air from which oxygen has been removed, or a rare gas, and the inert gas is humidified.
In step S2, the constant charging current is generated by a constant current source, a low potential point of the constant current source is connected to an anode end of the fuel cell stack into which hydrogen is introduced, a high potential point of the constant current source is connected to a cathode end of the fuel cell stack into which inert gas is introduced, and the number of the constant charging currents with different magnitudes is at least 3.
The step S2 specifically includes the following steps:
s21, setting a plurality of constant charging current values with different sizes, and setting a termination condition for the charging process;
s22, charging is started after the voltage of the galvanic pile or the voltage of each single battery in the galvanic pile is stabilized;
s23, applying constant charging current to the power pile through a constant current source, and cutting off the current charging current if a termination condition is triggered in the charging process;
s24, switching the charging current to the next set value according to the preset sequence or keeping the charging current unchanged;
and S25, repeating the steps S22-S24 until all the set charging work is finished.
In step S21, the termination condition includes:
(1) the cell voltage of a certain monomer in the electric pile reaches the termination voltage;
(2) the average voltage of all cells of the stack reaches the end voltage.
The termination voltage is set to be not more than 0.9V, so that the damage of the fuel cell monomer due to overhigh charging voltage is prevented.
The step S4 specifically includes the following steps:
s41, acquiring a voltage response curve according to the response voltage data of each single battery and the corresponding time data;
s42, an initial difference curve is obtained according to the voltage response curve, the initial difference curve is a relation curve of voltage change rate du/dt and time t, wherein u represents response voltage, the voltage change rate du/dt is obtained through a difference method, and a specific calculation formula is as follows:
where Δ u is a voltage variation, Δ t is a time variation, ut2And ut1Response voltages at the time t2 and the time t1 respectively, wherein t2 and t1 are two adjacent sampling times;
and S43, filtering the initial difference curve by adopting a filtering algorithm to obtain a corresponding difference curve.
In the step S5, each differential curve corresponds to a charging current, there is only one characteristic point on one differential curve, the characteristic point is specifically the last minimum value point before the differential curve reaches the highest point, and the characteristic point information is the voltage change rate at the time when the characteristic point corresponds to the point.
The step S6 specifically includes the following steps:
s61, selecting a single battery to be tested in the galvanic pile;
s62, extracting voltage change rate values corresponding to the characteristic points on the multiple differential curves and corresponding charging current values according to the voltage response data of the single battery;
s63, fitting the function model by using the extracted data and adopting a least square method, taking the fitting result of the model parameter n as the equivalent current value of the hydrogen permeation quantity in the single battery, wherein the expression of the function model is as follows:
y＝mx+n
wherein x is the voltage change rate of the characteristic point corresponding to the moment, y is the corresponding charging current, and m and n are model parameters;
and S64, repeating the steps S61-S63, and obtaining the equivalent current value of the hydrogen permeation quantity of all the single batteries to be tested.
In step S7, the conversion formula is specifically:
wherein F is the Faraday constant,
is an equivalent current value of the permeation amount of hydrogen gas,
the hydrogen permeation amount.
Compared with the prior art, the invention has the following advantages:
firstly, the test is accurate: the method can give quantitative results of the hydrogen permeation distribution of the monomers in the galvanic pile, accurately position the positions of the fault monomers, and has the test accuracy far higher than that of a hydrogen permeation qualitative detection method based on voltage change.
Secondly, the operability is strong: the hydrogen permeation measurement process of the method is carried out in a relatively stable gas environment, the test of the multi-section batteries of the galvanic pile can be carried out simultaneously, and the data processing rule is relatively clear.
Drawings
FIG. 1 is a schematic general flow diagram of the present invention.
FIG. 2 is a diagram illustrating exemplary voltage response signals under different charging currents in one embodiment.
Fig. 3 is an exemplary graph of a differential curve and its characteristic points under a specific charging current in the embodiment.
Fig. 4 is an exemplary graph of the hydrogen permeation amount results obtained by function model fitting in the examples.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments. Note that the following description of the embodiments is merely a substantial example, and the present invention is not intended to be limited to the application or the use thereof, and is not limited to the following embodiments.
As shown in fig. 1, the present embodiment provides a method for measuring hydrogen permeation amount of a fuel cell stack, the method comprising the steps of:
s1, introducing hydrogen into the anode side of the fuel cell stack, introducing inert gas into the cathode side, and keeping the pressure of the introduced gas on the two sides and the temperature of the fuel cell stack at constant levels;
s2, sequentially charging the fuel cell stacks by constant currents with different magnitudes;
s3, recording the voltage response of the fuel cell under each charging current;
s4, acquiring a differential curve of voltage response;
s5, extracting characteristic point information on the differential curve and a corresponding charging current value;
s6, fitting the function model by using the extracted data to obtain parameter values of the function model, and determining equivalent current of hydrogen permeation quantity in each single battery;
and S7, obtaining the hydrogen permeation amount in each single battery through conversion.
Examples
The test object of the present embodiment is a single proton exchange membrane fuel cell, but the actual application is not limited thereto.
The reaction area is 25cm2For the single fuel cell of (1), hydrogen gas is introduced into the anode, nitrogen gas is introduced into the cathode, and the temperature of the fuel cell is maintained at 60 ℃ and the gas pressure is 130 kPa.
The number of the charging currents is set to be 5, the magnitude of the charging currents is in the range of 175 mA-185 mA, the charging termination voltage is set to be 0.5V, the testing equipment collects time-varying voltage data of the fuel cell while applying constant charging current, when the voltage of the cell reaches the termination voltage, the equipment automatically cuts off the charging current, and the testing equipment automatically adjusts the charging current value according to a preset sequence before charging each time.
Fig. 2 is an exemplary diagram of battery voltage response curves under different charging currents, where an initial difference curve of the voltage response curves, a relation curve of voltage change rate du/dt and time t is obtained by a difference method, and the relationship curve is specifically calculated by the following formula:
where Δ u is a voltage variation, Δ t is a time variation, ut2And ut1The response voltages at the time t2 and the time t1, respectively, and t2 and t1 are two adjacent sampling times.
And filtering the initial difference curve by adopting a sliding filtering algorithm to obtain a corresponding difference curve, and determining the position of a characteristic point on the difference curve, namely the last minimum value point before du/dt reaches the highest point.
Fig. 3 is an exemplary graph of a differential curve and its characteristic points under a specific charging current, a voltage change rate value and a charging current value corresponding to the characteristic points on each differential curve are extracted, and a least square method is used to fit the extracted data and a function model, in this example, a linear function model is selected, and the expression is:
y＝mx+n
wherein x is the voltage change rate corresponding to the characteristic point, y is the corresponding charging current, and m and n are model parameters.
FIG. 4 is an exemplary graph of hydrogen permeation quantity results obtained by function model fitting, where the fitting result of the model parameter n is the equivalent current value of hydrogen permeation quantity
(0.1297A)。
Further, the hydrogen permeation amount is converted by the following formula, which includes:
wherein F is a Faraday constant (96485℃ mol)-1)，
The hydrogen permeation amount is expressed in mol · s-1。
The measurement result of the hydrogen permeation amount (6.721 × 10) was finally obtained-7mol·s-1)。
The above description is only exemplary of the present invention and should not be construed as limiting the invention, which is within the spirit and scope of the present invention.
Claims (10)
1. A method for measuring the hydrogen permeation quantity of a fuel cell stack is characterized by comprising the following steps:
s1, introducing hydrogen into the anode side of the fuel cell stack, introducing inert gas into the cathode side, and keeping the pressure of the introduced gas on the two sides and the temperature of the fuel cell stack at constant levels;
s2, sequentially charging the fuel cell stack by constant charging currents with different magnitudes;
s3, recording the voltage response of the fuel cell stack under each charging current;
s4, acquiring a differential curve of voltage response;
s5, extracting characteristic point information on the differential curve and a corresponding charging current value;
s6, fitting a function model according to the extracted feature point information and the charging current value to obtain parameter values of the function model, and determining equivalent current of hydrogen permeation quantity in each single battery;
and S7, obtaining the hydrogen permeation amount in each single battery through conversion.
2. The method as claimed in claim 1, wherein in step S1, the inert gas is nitrogen, air without oxygen, or a rare gas, and the inert gas is humidified.
3. The method as claimed in claim 1, wherein in step S2, the constant charging current is generated by a constant current source, a low potential point of the constant current source is connected to an anode end of the fuel cell stack through which hydrogen is introduced, a high potential point of the constant current source is connected to a cathode end of the fuel cell stack through which an inert gas is introduced, and the number of the constant charging currents with different magnitudes is at least 3.
4. The method as claimed in claim 3, wherein the step S2 specifically includes the following steps:
s21, setting a plurality of constant charging current values with different sizes, and setting a termination condition for the charging process;
s22, charging is started after the voltage of the galvanic pile or the voltage of each single battery in the galvanic pile is stabilized;
s23, applying constant charging current to the power pile through a constant current source, and cutting off the current charging current if a termination condition is triggered in the charging process;
s24, switching the charging current to the next set value according to the preset sequence or keeping the charging current unchanged;
and S25, repeating the steps S22-S24 until all the set charging work is finished.
5. A method for measuring the hydrogen permeation quantity of a fuel cell stack according to claim 3, wherein in step S21, the termination condition includes:
(1) the cell voltage of a certain monomer in the electric pile reaches the termination voltage;
(2) the average voltage of all cells of the stack reaches the end voltage.
6. The method of claim 5, wherein the end voltage is set to not more than 0.9V to prevent damage to the fuel cell unit due to excessive charging voltage.
7. The method for measuring the hydrogen permeation quantity of the fuel cell stack according to claim 1, wherein the step S4 specifically comprises the following steps:
s41, acquiring a voltage response curve according to the response voltage data of each single battery and the corresponding time data;
s42, an initial difference curve is obtained according to the voltage response curve, the initial difference curve is a relation curve of voltage change rate du/dt and time t, wherein u represents response voltage, the voltage change rate du/dt is obtained through a difference method, and a specific calculation formula is as follows:
where Δ u is a voltage variation, Δ t is a time variation, ut2And ut1Response voltages at the time t2 and the time t1 respectively, wherein t2 and t1 are two adjacent sampling times;
and S43, filtering the initial difference curve by adopting a filtering algorithm to obtain a corresponding difference curve.
8. The method as claimed in claim 1, wherein in step S5, each differential curve corresponds to a charging current, there is only one characteristic point on one differential curve, the characteristic point is a last minimum point before the differential curve reaches the highest point, and the characteristic point information is a voltage change rate at a time corresponding to the characteristic point.
9. The method for measuring the hydrogen permeation quantity of the fuel cell stack according to claim 1, wherein the step S6 specifically comprises the following steps:
s61, selecting a single battery to be tested in the galvanic pile;
s62, extracting voltage change rate values corresponding to the characteristic points on the multiple differential curves and corresponding charging current values according to the voltage response data of the single battery;
s63, fitting the function model by using the extracted data and adopting a least square method, taking the fitting result of the model parameter n as the equivalent current value of the hydrogen permeation quantity in the single battery, wherein the expression of the function model is as follows:
y＝mx+n
wherein x is the voltage change rate of the characteristic point corresponding to the moment, y is the corresponding charging current, and m and n are model parameters;
and S64, repeating the steps S61-S63, and obtaining the equivalent current value of the hydrogen permeation quantity of all the single batteries to be tested.
10. The method of claim 1, wherein in step S7, the conversion formula is specifically:
wherein F is the Faraday constant,
is an equivalent current value of the permeation amount of hydrogen gas,
the hydrogen permeation amount.
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| CN114976150A (en) * | 2022-06-21 | 2022-08-30 | 中国第一汽车股份有限公司 | Method, apparatus, device and medium for detecting single cell leakage in fuel cell stack |
| CN117250130A (en) * | 2023-11-20 | 2023-12-19 | 华电重工机械有限公司 | Proton exchange membrane hydrogen permeation testing method |
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| CN111525158A (en) * | 2020-06-04 | 2020-08-11 | 张家口市氢能科技有限公司 | Method and device for detecting physical state of air-cooled hydrogen fuel cell |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114976150A (en) * | 2022-06-21 | 2022-08-30 | 中国第一汽车股份有限公司 | Method, apparatus, device and medium for detecting single cell leakage in fuel cell stack |
| CN114976150B (en) * | 2022-06-21 | 2024-03-26 | 中国第一汽车股份有限公司 | Method, device, equipment and medium for detecting single cell leakage in fuel cell stack |
| CN117250130A (en) * | 2023-11-20 | 2023-12-19 | 华电重工机械有限公司 | Proton exchange membrane hydrogen permeation testing method |
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