CN113540524B - Aging quantification treatment method for proton exchange membrane fuel cell component - Google Patents

Aging quantification treatment method for proton exchange membrane fuel cell component Download PDF

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CN113540524B
CN113540524B CN202110704906.1A CN202110704906A CN113540524B CN 113540524 B CN113540524 B CN 113540524B CN 202110704906 A CN202110704906 A CN 202110704906A CN 113540524 B CN113540524 B CN 113540524B
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exchange membrane
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CN113540524A (en
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刘浩
陈剑
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Zhejiang University ZJU
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    • H—ELECTRICITY
    • 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
    • H01M8/04305—Modeling, demonstration models of fuel cells, e.g. for training purposes
    • H—ELECTRICITY
    • 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
    • H01M8/04537—Electric variables
    • H01M8/04544—Voltage
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • 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 discloses an aging quantification treatment method for a proton exchange membrane fuel cell component. The invention comprises the following steps: selecting a proton exchange membrane fuel cell, measuring operation performance parameters, and establishing a semi-mechanism voltage model of the proton exchange membrane fuel cell; measuring polarization curves of the fuel cell at different aging stages, fitting to obtain voltage model identification parameters corresponding to the different aging stages, and calculating total voltage polarization loss, sum of activation loss and permeation loss, total ohmic loss and total concentration loss under rated load in the different aging stages; respectively calculating the voltage loss caused by each component of the fuel cell in different aging stages by using a transmission line model; and calculating the voltage loss ratio caused by each component, and processing the fuel cell according to the aging quantification result of each component as the aging quantification result of each component. The invention realizes the aging quantification processing of the fuel cell components and improves the accuracy of the estimation of the aging state of the fuel cell.

Description

Aging quantification treatment method for proton exchange membrane fuel cell component
Technical Field
The invention belongs to an aging treatment method of a proton exchange membrane fuel cell in the field of research and development and application of fuel cells, and relates to an aging quantification treatment method of a proton exchange membrane fuel cell component.
Background
The aging of the proton exchange membrane fuel cell is a complex and strong nonlinear process, and involves complex factors such as multiple mechanisms, multiple components, multiple physical domains, multiple space-time scales, multiple working conditions and multiple couplings, so that the accurate and rapid estimation of the aging state becomes a great challenge. In addition, in the actual use process, the performance of the pem fuel cell recovers after shutdown and restart due to water management and other factors, which further increases the difficulty of estimating the aging state. At present, most fuel cell state estimation is based on macroscopic rough estimation of voltage, power, impedance or aging parameters (such as hydrogen permeability, catalyst electrochemical surface area and the like) of a single component, and the aging influence of specific different components on the whole fuel cell is unknown, which may cause great deviation of the fuel cell aging state estimation, and further influence the health operation and maintenance of the fuel cell. Taking voltage as an example, too many factors in design, production and use can affect the change in fuel cell voltage, not just aging. The voltage observed in practical use is reflected by the combined influence of various factors, inevitably contains a large amount of noise and fluctuation, and is likely to deviate when the aging state of the fuel cell is estimated from the voltage. After the quantitative information of the influence of each component on the aging of the whole fuel cell is known, the aging state of the fuel cell can be accurately estimated, and a targeted prediction operation and maintenance method is further adopted. Therefore, the research on the aging quantification treatment method of the proton exchange membrane fuel cell component is of great significance.
The polarization curve fitting and the transmission line model are widely applied to the directions of mechanism disclosure, modeling simulation and the like of the proton exchange membrane fuel cell for years, and are an effective method capable of quantitatively processing the performance of fuel cell components. However, the application of this set of methods to the analysis of the impact of processing different components at different stages of aging on the overall fuel cell aging has not been investigated.
Disclosure of Invention
In order to solve the defects of the prior art, the invention provides an aging quantification treatment method for a proton exchange membrane fuel cell component.
The scheme adopted by the invention is as follows:
the invention comprises the following steps:
1) selecting a brand-new proton exchange membrane fuel cell, measuring the operation performance parameters of the fuel cell under rated load and standard operation conditions, and establishing a semi-mechanism voltage model of the proton exchange membrane fuel cell according to the operation performance parameters of the fuel cell;
2) measuring polarization curves of the fuel cell in different aging stages under standard operation conditions, fitting the polarization curves of the fuel cell in the different aging stages by using a semi-mechanism voltage model to obtain voltage model identification parameters corresponding to the different aging stages, and calculating total voltage polarization loss, sum of activation loss and permeation loss, total ohmic loss and total concentration loss of the fuel cell in the different aging stages under rated load according to the voltage model identification parameters corresponding to the different aging stages;
3) Respectively calculating the voltage loss caused by each component of the fuel cell in different aging stages by utilizing a transmission line model according to the total voltage polarization loss, the sum of the activation loss and the penetration loss, and the total ohmic loss and the total concentration loss of the fuel cell in different aging stages;
4) and dividing the voltage loss caused by each component of the fuel cell in different aging stages under the rated load by the total polarization loss of the voltage corresponding to the aging stages, calculating to obtain the voltage loss ratio caused by each component in different aging stages, and taking the ratio as the aging quantification result of each component in different aging stages, thereby judging the overall aging state of the fuel cell and processing the fuel cell.
The semi-mechanism voltage model of the proton exchange membrane fuel cell in the step 1) is set through a formula:
Ecell＝Ener-ηact+cross-ηohmic-ηcon
wherein, EcellIndicating the cell voltage of the monolithic fuel cell, EnerIndicating the nernst voltage, eta, of a monolithic fuel cellact+crossRepresenting the sum of the activation loss and the permeation loss, η, of a monolithic fuel cellohmicRepresenting the total ohmic loss, eta, of the monolithic fuel cellconRepresenting the total concentration loss of the monolithic fuel cell.
The sum eta of activation loss and penetration loss of the monolithic fuel cell act+crossThe setting is made by the following formula:
Figure BDA0003131794290000021
Figure BDA0003131794290000022
wherein, AcDenotes the activation constant, i, of the cathodecrossDenotes an infiltration current density, i denotes a rated load current density, a constant 10 is a unit conversion factor, f denotes a catalyst roughness factor, and f is ECSA × LptECSA is the electrochemical surface area of the platinum catalyst, LptRepresents the platinum loading of the cathode, i0,cRepresents the cathode exchange current density;
Figure BDA0003131794290000023
denotes the reference partial pressure, T, of the cathodic oxygen under standard operating conditionsrefA reference operating temperature of the fuel cell is indicated,
Figure BDA0003131794290000024
is shown in
Figure BDA0003131794290000025
And TrefA reference value of the cathode exchange current density at operating conditions,
Figure BDA0003131794290000026
denotes the partial pressure of oxygen, gamma, of the cathodecRepresenting the reaction order of the oxygen reduction reaction, Eact,cRepresents the activation energy of the oxygen reduction reaction; r represents an ideal gas constant; t represents a fuel cell operating temperature;
total ohmic loss η of the monolithic fuel cellohmicThe setting is made by the following formula:
ηohmic＝iRohmic
Figure BDA0003131794290000027
wherein R isohmicDenotes the total ohmic resistance, RmRepresents the proton transport resistance of the proton exchange membrane,
Figure BDA0003131794290000028
represents the effective proton transport resistance, R, of the cathode catalyst layerctRepresents the contact resistance between the bipolar plate and the gas diffusion layer;
total concentration loss η of the monolithic fuel cellconThe setting is made by the following formula:
Figure BDA0003131794290000031
Wherein, BcDenotes the concentration constant, i, of the cathodelimIndicating the limiting current density.
The step 3) is specifically as follows:
the fuel cell mainly comprises a catalyst layer, a proton exchange membrane, a bipolar plate and a gas diffusion layer;
s1: respectively calculating the activation loss and the penetration loss according to the sum of the activation loss and the penetration loss, wherein the activation loss is completely caused by a catalyst layer of the fuel cell, and the penetration loss is completely caused by a proton exchange membrane of the fuel cell;
wherein the activation loss and the permeation loss of the monolithic fuel cell are calculated by the following formulas:
Figure BDA0003131794290000032
Figure BDA0003131794290000033
wherein eta isactRepresents the activation loss, η, of a monolithic fuel cellcrossRepresents the permeation loss of a monolithic fuel cell; i.e. icrossRepresents the percolation current density; i represents a rated load current density; etaact+crossRepresents the sum of the activation loss and the permeation loss of the monolithic fuel cell;
s2: the total ohmic loss is respectively caused by a proton exchange membrane, a catalyst layer and a bipolar plate of the fuel cell, and according to the total ohmic loss, a transmission line model is utilized to respectively calculate the proton transmission resistance of the proton exchange membrane, the effective proton transmission resistance of a cathode catalyst layer and the contact resistance between the bipolar plate and a gas diffusion layer, so that the ohmic loss caused by the proton exchange membrane, the ohmic loss caused by the catalyst layer and the ohmic loss caused by the bipolar plate are calculated;
Wherein the proton transfer resistance R of the proton exchange membrane of the single-chip fuel cellmThe calculation formula is as follows:
Figure BDA0003131794290000034
wherein, deltam,dryThe thickness of the dry proton exchange membrane is expressed,
Figure BDA0003131794290000035
represents the effective proton conductivity, δ, of the proton exchange membraneswellThe expansion ratio of the proton exchange membrane after water absorption is expressed;
effective proton transport resistance of cathode catalyst layer of monolithic fuel cell
Figure BDA0003131794290000036
The calculation formula of (2) is as follows:
Figure BDA0003131794290000037
wherein the content of the first and second substances,
Figure BDA0003131794290000038
is the proton transport resistance of the catalytic layer, constant 3 indicates that protons react with oxygen at the interface of the catalytic layer and the gas diffusion layer, ζ is a correction factor that takes into account the effect of oxygen transport limitation;
contact resistance R between bipolar plate and gas diffusion layer of monolithic fuel cellctThe calculation method of (2) is as follows:
Figure BDA0003131794290000039
s3: the total concentration loss is caused by a gas diffusion layer and a catalyst layer of the fuel cell, and according to the total concentration loss of the fuel cell, the average liquid water saturation of the gas diffusion layer and the average liquid water saturation of the catalyst layer are reversely calculated by using a transmission line model to obtain the oxygen transmission resistance of the gas diffusion layer and the catalyst layer, so that the concentration loss caused by the gas diffusion layer and the catalyst layer respectively is obtained;
wherein the oxygen transmission resistances of the gas diffusion layer and the catalytic layer of the monolithic fuel cell are set by the following formula:
Figure BDA0003131794290000041
Wherein, the first and the second end of the pipe are connected with each other,
Figure BDA0003131794290000042
represents the total resistance to oxygen transport of the cathode of a monolithic fuel cell,
Figure BDA0003131794290000043
which represents the resistance to oxygen transport in the monolithic fuel cell cathode flow channel to gas diffusion layer interface,
Figure BDA0003131794290000044
representing the resistance to oxygen transport in the gas diffusion layer of the cathode of the monolithic fuel cell,
Figure BDA0003131794290000045
which represents the resistance to oxygen transport in the cathode catalytic layer of a monolithic fuel cell,
Figure BDA0003131794290000046
represents the local resistance of oxygen transmission in the cathode catalytic layer of the single fuel cell;
Figure BDA0003131794290000047
the resistance to oxygen transmission caused by the gas diffusion layer,
Figure BDA0003131794290000048
oxygen transport resistance due to the catalytic layer;
the concentration losses caused by the gas diffusion layer and the catalytic layer, respectively, are set by the following equations:
Figure BDA0003131794290000049
Figure BDA00031317942900000410
wherein eta iscon1Concentration loss, η, caused by gas diffusion layerscon2Concentration loss for the catalytic layer;
s4: and calculating the voltage loss caused by each component of the fuel cell in different aging stages according to the activation loss, the penetration loss, the ohmic loss and the concentration loss caused by each component in the steps S1-S3, wherein the voltage loss caused by the proton exchange membrane is the sum of the penetration loss of the fuel cell and the ohmic loss of the proton exchange membrane, the voltage loss caused by the catalytic layer is the sum of the activation loss of the fuel cell, the ohmic loss of the catalytic layer and the concentration loss of the catalytic layer, the voltage loss caused by the gas diffusion layer is the concentration loss of the gas diffusion layer, and the voltage loss caused by the bipolar plate is the ohmic loss of the bipolar plate.
The voltage total polarization loss is the sum of activation loss, penetration loss, total ohmic loss and total concentration loss.
The beneficial effects of the invention are:
the invention solves the problem of quantitative processing of the aging of the proton exchange membrane fuel cell components, also solves the problem of difficult estimation of the aging state of the fuel cell caused by the influence of the performance recovery phenomenon, can improve the accuracy of the estimation of the aging state of the proton exchange membrane fuel cell, further constructs better aging parameters to improve the healthy operation and maintenance effect of the fuel cell, and prolongs the service life of the fuel cell. The obtained average liquid water content parameter can also be used for diagnosing whether water management faults occur in the fuel cell, and the reliability and the durability of the fuel cell are improved.
Drawings
FIG. 1 is a schematic view of the component structure of a PEM fuel cell according to the present invention.
FIG. 2 is a flow chart of the aging quantification method of the PEMFC component according to the present invention.
FIG. 3 is a polarization curve of a PEM fuel cell according to an embodiment of the present invention during different stages of aging under standard operating conditions.
FIG. 4 is a graph of the fitting result of the polarization curve based on the half-mechanism voltage model of the PEM fuel cell in the embodiment of the present invention.
Detailed Description
The present invention will be described in detail below with reference to specific embodiments shown in the drawings.
As shown in fig. 2, the present invention comprises the steps of:
1) selecting a brand-new proton exchange membrane fuel cell, and measuring the operation performance parameters of the fuel cell under rated load and standard operation conditions, wherein the operation performance parameters comprise electrochemical surface area, permeation current density, exchange current density, contact resistance and limiting current density; establishing a semi-mechanism voltage model of the proton exchange membrane fuel cell according to the operation performance parameters of the fuel cell;
the semi-mechanism voltage model of the proton exchange membrane fuel cell in the step 1) is set through a formula:
Ecell＝Ener-ηact+cross-ηohmic-ηcon
wherein E iscellIndicating the cell voltage of the monolithic fuel cell, EnerIndicating the nernst voltage, η, of a monolithic fuel cellact+crossRepresenting the sum of the activation loss and the permeation loss, η, of a monolithic fuel cellohmicRepresenting the total ohmic loss, η, of the monolithic fuel cellconRepresenting the total concentration loss of the monolithic fuel cell. The proton exchange membrane fuel cell is formed by connecting a plurality of single fuel cells in series, and the structural schematic diagram of the single fuel cell is shown in fig. 1.
Due to the rapid oxidation reaction and high diffusion rate of hydrogen in the anode catalytic layer and the gas diffusion layer of the fuel cell, activation loss, permeation loss and concentration loss on the anode can be ignored. The contact resistance between the catalyst layer and the gas diffusion layer of the fuel cell and the contact resistance between the catalyst layer and the proton exchange membrane are smaller than the contact resistance between the gas diffusion layer and the bipolar plate by more than one order of magnitude and can be ignored. Since each component of the fuel cell has larger electrical conductivity, the bulk resistance of different components can be ignored, and the total ohmic resistance only needs to consider the transfer resistance of protons in the membrane, the effective transfer resistance of protons in the cathode catalyst layer and the contact resistance between the gas diffusion layer and the bipolar plate.
Inster voltage parameter E of monolithic fuel cellnerThe calculation formula of (2) is as follows:
Figure BDA0003131794290000051
wherein T represents the fuel cell operating temperature, R represents an ideal gas constant, F represents a Faraday constant,
Figure BDA0003131794290000061
and
Figure BDA0003131794290000062
respectively representing the hydrogen partial pressure at the anode and the oxygen partial pressure at the cathode,
Figure BDA0003131794290000063
and
Figure BDA0003131794290000064
reference partial pressures for anode hydrogen and cathode oxygen are indicated, respectively, under standard operating conditions. During the actual operation of the fuel cell, the T and the T are kept as much as possible,
Figure BDA0003131794290000065
And
Figure BDA0003131794290000066
is constant, therefore EnerCan be considered as a constant.
Sum of activation loss and permeation loss eta of monolithic fuel cellact+crossThe setting is made by the following formula:
Figure BDA0003131794290000067
Figure BDA0003131794290000068
wherein A iscDenotes the activation constant of the cathode, activation constant A of the cathodecObtained by fitting a polarization curve of an initial aging stage in each of which the activation constant of the cathode remains constant, icrossDenotes an infiltration current density, i denotes a rated load current density, a constant 10 is a unit conversion factor, f denotes a catalyst roughness factor, and f ═ ECSA × L is satisfiedptECSA is the electrochemical surface area of the platinum catalyst, LptRepresents the platinum loading of the cathode, i0,cRepresents the cathode exchange current density;
Figure BDA0003131794290000069
is shown in
Figure BDA00031317942900000610
And TrefA reference value of the cathode exchange current density at operating conditions,
Figure BDA00031317942900000611
denotes the reference partial pressure, T, of the cathodic oxygen under standard operating conditions refA reference operating temperature of the fuel cell is indicated,
Figure BDA00031317942900000612
denotes the partial pressure of oxygen, gamma, of the cathodecRepresenting the reaction order of the oxygen reduction reaction, Eact,cMeans oxygen reductionThe activation energy of the original reaction; r represents an ideal gas constant; t represents a fuel cell operating temperature;
total ohmic loss eta of monolithic fuel cellohmicThe setting is made by the following formula:
ηohmic＝iRohmic
Figure BDA00031317942900000613
wherein R isohmicDenotes the total ohmic resistance, RmRepresents the proton transport resistance of the proton exchange membrane,
Figure BDA00031317942900000614
represents the effective proton transport resistance, R, of the cathode catalyst layerctRepresents the contact resistance between the bipolar plate and the gas diffusion layer;
total concentration loss eta of monolithic fuel cellconThe setting is made by the following formula:
Figure BDA00031317942900000615
wherein, BcRepresenting the concentration constant of the cathode, obtained by fitting a polarization curve of an initial aging stage in which the concentration constant of the cathode remains constant, ilimIndicating the limiting current density.
2) Under standard operating conditions, polarization curves of the fuel cell at different aging stages are measured, as shown in fig. 3, a semi-mechanism voltage model is used to fit the polarization curves at different aging stages, as shown in fig. 4, a least square fitting method is used in the present example, to obtain voltage model identification parameters corresponding to different aging stages, and the voltage model identification parameters include a cathode activation constant, a cathode concentration constant, a total ohmic resistance, a product of a catalyst roughness factor and a cathode exchange current density, a limiting current density, and a permeation current density, as shown in table 1. Calculating the total voltage polarization loss, the sum of activation loss and permeation loss, the total ohmic loss and the total concentration loss of the fuel cell in different aging stages under rated load according to the voltage model identification parameters corresponding to the different aging stages; the rated load is the rated load current density. The total voltage polarization loss is the sum of the activation loss, the permeation loss, the total ohmic loss and the total concentration loss, and in this example, the total voltage polarization loss, the sum of the activation loss and the permeation loss, the total ohmic loss and the total concentration loss of the fuel cell under the rated load are obtained by fitting, as shown in table 2.
Parameter identification results of proton exchange membrane fuel cell semi-mechanism voltage model in table 1 after fitting polarization curves of different aging stages
Figure BDA0003131794290000071
TABLE 2 Total voltage polarization loss, sum of activation loss and permeation loss, total ohmic loss and total concentration loss of PEM fuel cells at different aging stages under rated load in example 2
Figure BDA0003131794290000072
3) Respectively calculating the voltage loss caused by each component of the fuel cell in different aging stages by using a transmission line model according to the total voltage polarization loss, the sum of the activation loss and the permeation loss, and the total ohmic loss and the total concentration loss of the fuel cell in different aging stages;
the step 3) is specifically as follows:
the fuel cell mainly comprises a catalyst layer, a proton exchange membrane, a bipolar plate and a gas diffusion layer;
s1: respectively calculating the activation loss and the penetration loss according to the sum of the activation loss and the penetration loss, wherein the activation loss is completely caused by a catalyst layer of the fuel cell, and the penetration loss is completely caused by a proton exchange membrane of the fuel cell;
wherein the activation loss and the permeation loss of the monolithic fuel cell are calculated by the following formulas:
Figure BDA0003131794290000081
Figure BDA0003131794290000082
wherein eta isactRepresents the activation loss, η, of a monolithic fuel cell crossRepresents the permeation loss of a monolithic fuel cell; i all right anglecrossRepresents the percolation current density; i represents a rated load current density; etaact+crossRepresents the sum of the activation loss and the permeation loss of the monolithic fuel cell;
i0,caffected by the cathode oxygen partial pressure and the fuel cell operating temperature. Since the actual fuel cell will try to keep the two operating parameters stable during use, it can be assumed that i0,cIs a constant during the aging of the fuel cell. The product f multiplied by i of the catalyst roughness factor and the cathode exchange current density in the voltage model identification parameters can be obtained according to the polarization curve fitting in the previous step0,cValue divided by i0,cAnd f values of the fuel cell in different aging stages are calculated.
Research has shown that the permeation current density i is measured during the aging process of the fuel cell when the proton exchange membrane is not cracked or perforated due to chemical degradation, mechanical degradation, thermal degradation and the likecrossFluctuation in a very small range, which can be regarded as a constant, i if the film is perforated or brokencrossA sharp increase in non-linearity is initiated. The specific calculation method is as follows:
Figure BDA0003131794290000083
Vb＝V0-0.632×(V0-VL)
wherein r isicrossRepresents icrossIncreased proportion of V relative to the initial valuebRepresents the critical voltage point of the fuel cell under rated load, and is used for comparing with the critical voltage point E under rated load cellComparing to determine whether i is reachedcrossCritical point of change, V0Denotes the initial monolithic voltage value at the rated load of the fuel cell, A denotes Ecell≤VbAverage decay rate of voltage of fuel cell sheet, VLIndicates the initial single-chip voltage value V under the rated load of the fuel cell0The value after 10% decay, t represents the aging time.
S2: the total ohmic loss is respectively caused by a proton exchange membrane, a catalyst layer and a bipolar plate of the fuel cell, and according to the total ohmic loss, a transmission line model is utilized to respectively calculate the proton transmission resistance of the proton exchange membrane, the effective proton transmission resistance of a cathode catalyst layer and the contact resistance between the bipolar plate and a gas diffusion layer, so that the ohmic loss caused by the proton exchange membrane, the ohmic loss caused by the catalyst layer and the ohmic loss caused by the bipolar plate are calculated;
wherein, the proton transmission resistance R of the proton exchange membrane of the monolithic fuel cellmThe calculation formula is as follows:
Figure BDA0003131794290000084
wherein, deltam,dryRepresents the thickness, δ, of the dry proton exchange membranem,wetThe thickness of the wet proton exchange membrane is shown,
Figure BDA0003131794290000091
represents the effective proton conductivity, δ, of the proton exchange membraneswellThe expansion ratio of the proton exchange membrane after absorbing water is expressed;
thickness delta of the proton exchange membrane during aging of the proton exchange membrane m,wetAnd effective proton conductivity
Figure BDA0003131794290000092
Will be reduced, and the practical experiment result shows that the proton transmission resistance R of the proton exchange membranemThe change with the aging of the proton exchange membrane is not large, and the change is usually less than 10 percent, which can be ignored. During actual fuel cell aging, R can be assumed before the proton exchange membrane does not crack or perforatemIs a constant.
Effective proton transport resistance of cathode catalyst layer of monolithic fuel cell
Figure BDA0003131794290000093
The calculation formula of (2) is as follows:
Figure BDA0003131794290000094
wherein the content of the first and second substances,
Figure BDA0003131794290000095
is the proton transport resistance of the catalytic layer, constant 3 indicates that protons react with oxygen at the interface of the catalytic layer and the gas diffusion layer, ζ is a correction factor that takes into account the effect of oxygen transport limitation;
it has been shown that the proton transfer resistance of the catalytic layer is an inherent property of the catalytic layer, regardless of the platinum loading and the catalytic layer thickness, and neither ordinary catalytic layer aging nor severe carbon corrosion causes
Figure BDA0003131794290000096
Compared with the concentration loss caused by the increase of oxygen transmission resistance caused by the aging of the catalytic layer,
Figure BDA0003131794290000097
the change in total ohmic losses due to the change is negligible. In the course of the actual ageing of the fuel cell,
Figure BDA0003131794290000098
or may be considered a constant.
Contact resistance R between bipolar plate and gas diffusion layer of monolithic fuel cell ctThe calculation method of (2) is as follows:
Figure BDA0003131794290000099
in the invention, R isctThe resulting ohmic losses are all attributed to the bipolar plate.
S3: the total concentration loss is respectively caused by a gas diffusion layer and a catalyst layer of the fuel cell, and according to the total concentration loss of the fuel cell, the average liquid water saturation of the gas diffusion layer and the average liquid water saturation of the catalyst layer are reversely calculated by using a transmission line model to obtain the oxygen transmission resistance of the gas diffusion layer and the catalyst layer, so that the concentration loss respectively caused by the gas diffusion layer and the catalyst layer is obtained;
wherein the oxygen transmission resistances of the gas diffusion layer and the catalytic layer of the monolithic fuel cell are set by the following formula:
Figure BDA00031317942900000910
wherein, the first and the second end of the pipe are connected with each other,
Figure BDA00031317942900000911
represents the total resistance to oxygen transport of the cathode of a monolithic fuel cell,
Figure BDA00031317942900000912
which represents the resistance to oxygen transport in the monolithic fuel cell cathode flow channel to gas diffusion layer interface,
Figure BDA00031317942900000913
representing the resistance to oxygen transport in the gas diffusion layer of the cathode of the monolithic fuel cell,
Figure BDA00031317942900000914
which represents the resistance to oxygen transport in the cathode catalytic layer of a monolithic fuel cell,
Figure BDA00031317942900000915
representing oxygen transport in the cathode catalytic layer of a monolithic fuel cellThe local resistance is the local resistance of the water,
Figure BDA00031317942900000916
containing the resistance to the transmission of oxygen in the carbon paper layer
Figure BDA00031317942900000917
And resistance to oxygen transport in the microporous layer
Figure BDA00031317942900000918
Two parts;
Figure BDA00031317942900000919
the resistance to oxygen transmission caused by the gas diffusion layer,
Figure BDA0003131794290000101
Oxygen transport resistance due to the catalytic layer;
the concentration loss caused by each of the gas diffusion layer and the catalytic layer is set by the following formula:
Figure BDA0003131794290000102
Figure BDA0003131794290000103
wherein etacon1Concentration loss, eta, caused by gas diffusion layerscon2Concentration loss due to the catalytic layer.
After the total oxygen transmission resistance of the cathode of the fuel cell is obtained through calculation, the total concentration loss of the fuel cell caused by the total oxygen transmission resistance is calculated by the following formula:
Figure BDA0003131794290000104
in calculating the loss of components in the total concentration loss of a fuel cell, it is assumed that the liquid water saturation in the catalytic layer and the gas diffusion layer is uniformly distributedIs represented as savg. Substituting the total concentration loss value obtained by the polarization curve fitting in the step 2) into a formula, calculating the average liquid water saturation in the catalytic layer and the gas diffusion layer through reverse derivation, and further calculating to obtain the concentration loss caused by each component.
(a) Oxygen transport resistance in fuel cell cathode flow channel and gas diffusion layer interface
Figure BDA0003131794290000105
The calculation formula of (c) is as follows:
Figure BDA0003131794290000106
where Sh denotes the Sherwood constant, DhThe diameter of the water flow in the flow channel is shown,
Figure BDA0003131794290000107
the diffusivity of oxygen in the carbon paper layer is expressed, and the calculation formula is as follows:
Figure BDA0003131794290000108
wherein the content of the first and second substances,
Figure BDA0003131794290000109
is the binary diffusivity of oxygen in nitrogen,
Figure BDA00031317942900001010
is the Knuden diffusivity of oxygen in the carbon paper layer, and the calculation formula of the Knuden diffusivity and the Knuden diffusivity is as follows:
Figure BDA00031317942900001011
Figure BDA00031317942900001012
Wherein p iscDenotes the gas pressure of the cathode of the fuel cell, rKn,CBPRepresenting the Knuden radius of the carbon paper layer,
Figure BDA00031317942900001013
represents the molar mass of oxygen.
(b) Oxygen transport resistance in carbon paper layer of cathode gas diffusion layer of fuel cell
Figure BDA0003131794290000111
The calculation formula of (a) is as follows:
Figure BDA0003131794290000112
wherein, deltaCBPWhich represents the thickness of the carbon paper layer in the gas diffusion layer of the fuel cell,
Figure BDA0003131794290000113
the effective diffusion rate of oxygen in the carbon paper layer is represented by the following calculation formula:
Figure BDA0003131794290000114
wherein epsilonCBPDenotes the porosity, s, of the carbofrax layeravgRepresents the average liquid water saturation of the carbon paper layer, f (epsilon)CBP) And f(s)avg) Respectively representing porosity and average liquid water saturation correction factors, and calculating the formula as follows:
Figure BDA0003131794290000115
Figure BDA0003131794290000116
wherein n iseAnd nvAre fitting parameters.
(c) Fuel cell cathode gasOxygen transport resistance in microporous layers of diffusion layers
Figure BDA0003131794290000117
The calculation formula of (a) is as follows:
Figure BDA0003131794290000118
wherein, deltaMPLWhich represents the thickness of the microporous layer in the gas diffusion layer of the fuel cell,
Figure BDA0003131794290000119
representing the effective diffusivity of oxygen in the microporous layer, a desired parameter is Knuden diffusivity of oxygen in the microporous layer
Figure BDA00031317942900001110
Knuden radius r of microporous layerKn,MPLPorosity epsilon of microporous layerMPLAverage liquid water saturation s of microporous layeravg。
(d) Oxygen transport resistance in fuel cell cathode catalyst layer
Figure BDA00031317942900001111
The calculation formula of (a) is as follows:
Figure BDA00031317942900001112
wherein, delta CLWhich represents the thickness of the catalytic layer of the fuel cell,
Figure BDA00031317942900001113
the required parameter is Knuden diffusivity of oxygen in the catalytic layer
Figure BDA00031317942900001114
Knuden radius r of the catalytic layerKn,CLPorosity of the catalytic layer εCLAverage liquid water saturation s of the catalytic layeravg。
(e) Local oxygen transport resistance in fuel cell cathode catalyst layer
Figure BDA00031317942900001115
The calculation formula of (a) is as follows:
Figure BDA00031317942900001116
wherein R isw,dissRepresents the resistance to oxygen transmission, R, due to the dissolution of oxygen in waterw,diffRepresenting the resistance to oxygen transmission, R, due to oxygen passing through the water filmion,dissDenotes the resistance to oxygen transmission, R, due to the dissolution of oxygen in the polymerion,diffIndicating the resistance to oxygen transmission due to oxygen passing through the polymer film,
Figure BDA00031317942900001117
indicating the resistance to oxygen transfer due to adsorption of oxygen by the active platinum catalyst.
Oxygen transmission resistance R caused by dissolution in waterw,dissThe calculation method is as follows:
Figure BDA0003131794290000121
wherein k is1Is the fitting constant, δwThe thickness of the liquid water film on the surface of the active platinum particles is shown,
Figure BDA0003131794290000122
the binary diffusivity of oxygen in liquid water is represented, and the specific calculation formula is as follows:
Figure BDA0003131794290000123
Figure BDA0003131794290000124
wherein psiwDenotes the association parameter of water,. mu.wWhich represents the viscosity of the water and is,
Figure BDA0003131794290000125
represents the molar volume of oxygen, rCDenotes the radius, ε, of the carbon support particles in the catalyst CRepresenting the volume fraction, delta, of carbon in the catalytic layerionThe thickness of the polymer film on the surface of the active platinum particles is represented by the following specific calculation formula:
Figure BDA0003131794290000126
Figure BDA0003131794290000127
wherein ρCDenotes the density of carbon, LCRepresenting the carbon loading in the catalyst, wt% representing the mass fraction of platinum relative to carbon, epsilonionThe volume fraction of the polymer is expressed by the following formula:
εion＝0.2×I/C
wherein I/C represents the ratio of polymer to carbon.
Oxygen transmission resistance R through water filmw,diffThe calculation method is as follows:
Figure BDA0003131794290000128
resistance to oxygen transmission R caused by dissolution in polymersion,dissThe calculation method is as follows:
Figure BDA0003131794290000129
wherein k is2Is the constant of the fit, and,
Figure BDA00031317942900001210
the binary diffusivity of oxygen in the polymer is expressed, and the specific calculation formula is as follows:
Figure BDA00031317942900001211
wherein f isvThe volume fraction of water in the polymer film is expressed by the following formula:
Figure BDA00031317942900001212
oxygen transmission resistance R through polymer filmion,diffThe calculation method is as follows:
Figure BDA0003131794290000131
oxygen transport resistance due to adsorption of active platinum catalyst
Figure BDA0003131794290000132
The calculation method is as follows:
Figure BDA0003131794290000133
wherein k is3Is the fitting constant.
Parameters such as average liquid water saturation, catalyst roughness factor, cathode exchange current density, proton transfer resistance of a proton exchange membrane, effective proton transfer resistance of a cathode catalyst layer, contact resistance of a gas diffusion layer and a bipolar plate, oxygen transfer resistance in the catalyst layer, oxygen transfer resistance in the gas diffusion layer and the like are obtained in the embodiment of the invention, and are shown in tables 3 and 4.
TABLE 3 shows the parameters of the components corresponding to the activation loss and the total ohmic loss of the PEM fuel cell at different aging stages under rated load
Figure BDA0003131794290000134
TABLE 4 example of the relevant parameters of each component corresponding to the total concentration loss of the PEM fuel cell at different aging stages under rated load
Figure BDA0003131794290000135
S4: and calculating the voltage loss of each component of the fuel cell in different aging stages according to the activation loss, the penetration loss, the ohmic loss and the concentration loss caused by each component in the steps S1-S3, wherein the voltage loss caused by the proton exchange membrane is the sum of the penetration loss of the fuel cell and the ohmic loss of the proton exchange membrane, the voltage loss caused by the catalytic layer is the sum of the activation loss of the fuel cell, the ohmic loss of the catalytic layer and the concentration loss of the catalytic layer, the voltage loss caused by the gas diffusion layer is the concentration loss of the gas diffusion layer, and the voltage loss caused by the bipolar plate is the ohmic loss of the bipolar plate.
4) The voltage loss caused by each component of the fuel cell in different aging stages under rated load is divided by the total polarization loss of the voltage corresponding to the aging stage, the voltage loss ratio of each component in different aging stages is calculated and obtained and is used as the aging quantification result of each component in different aging stages, as shown in table 5, so that the aging state of the whole fuel cell is judged and the fuel cell is processed. Based on the aging quantification results of the components, the aging characteristics of the whole fuel cell can be further constructed by fusing the aging parameters of the components, such as the catalyst roughness factor f of the catalyst layer and the permeation current density i of the proton exchange membrane crossThereby more accurately characterizing the aging state of the fuel cell and further adopting a proper method to increase the service life of the fuel cell.
TABLE 5 results of quantifying the aging of various components of PEM fuel cells at different aging stages under rated load in the examples
Aging stage Proton exchange membrane Catalytic layer Gas diffusion layer Bipolar plate
0h 0.0598 0.8575 0.0351 0.0476
48h 0.0594 0.8563 0.0362 0.0481
185h 0.0585 0.8536 0.0386 0.0493
348h 0.0580 0.8522 0.0389 0.0509
515h 0.0576 0.8490 0.0397 0.0537
658h 0.0572 0.8472 0.0405 0.0551
823h 0.0565 0.8443 0.0419 0.0573

Claims (5)

1. A method for quantifying the aging of a proton exchange membrane fuel cell component, comprising the steps of:
1) selecting a brand-new proton exchange membrane fuel cell, measuring the operation performance parameters of the fuel cell under rated load and standard operation conditions, and establishing a semi-mechanism voltage model of the proton exchange membrane fuel cell according to the operation performance parameters of the fuel cell;
2) measuring polarization curves of the fuel cell in different aging stages under standard operation conditions, fitting the polarization curves of the fuel cell in the different aging stages by using a semi-mechanism voltage model to obtain voltage model identification parameters corresponding to the different aging stages, and calculating total voltage polarization loss, sum of activation loss and permeation loss, total ohmic loss and total concentration loss of the fuel cell in the different aging stages under rated load according to the voltage model identification parameters corresponding to the different aging stages;
3) Respectively calculating the voltage loss caused by each component of the fuel cell in different aging stages by utilizing a transmission line model according to the total voltage polarization loss, the sum of the activation loss and the penetration loss, and the total ohmic loss and the total concentration loss of the fuel cell in different aging stages;
4) and dividing the voltage loss caused by each component of the fuel cell in different aging stages under the rated load by the total voltage polarization loss in the corresponding aging stage, calculating to obtain the voltage loss ratio caused by each component in different aging stages, and taking the ratio as the aging quantization result of each component in different aging stages, thereby judging the overall aging state of the fuel cell and processing the fuel cell.
2. The method as claimed in claim 1, wherein the semi-mechanism voltage model of the pem fuel cell in step 1) is set by the following formula:
Ecell＝Ener-ηact+cross-ηohmic-ηcon
wherein, EcellIndicating the cell voltage of the monolithic fuel cell, EnerIndicating the nernst voltage, eta, of a monolithic fuel cellact+crossRepresenting the sum of the activation loss and the permeation loss, η, of a monolithic fuel cellohmicRepresenting the total ohmic loss, η, of the monolithic fuel cell conRepresenting the total concentration loss of the monolithic fuel cell.
3. The method according to claim 2, wherein the aging process of the PEMFC component is performed by a single step,
the sum eta of activation loss and penetration loss of the single-chip fuel cellact+crossThe setting is made by the following formula:
Figure FDA0003131794280000011
Figure FDA0003131794280000021
wherein A iscDenotes the activation constant, i, of the cathodecrossDenotes an infiltration current density, i denotes a rated load current density, a constant 10 is a unit conversion factor, f denotes a catalyst roughness factor, and f ═ ECSA × L is satisfiedptECSA is the electrochemical surface area of the platinum catalyst, LptRepresents the platinum loading of the cathode, i0,cRepresents the cathode exchange current density;
Figure FDA0003131794280000022
denotes the reference partial pressure, T, of the cathodic oxygen under standard operating conditionsrefA reference operating temperature of the fuel cell is indicated,
Figure FDA0003131794280000023
is shown in
Figure FDA0003131794280000024
And TrefReference value, p, of the cathode exchange current density under operating conditionsO2Denotes the partial pressure of oxygen, gamma, of the cathodecRepresenting the reaction order of the oxygen reduction reaction, Eact,cRepresents the activation energy of the oxygen reduction reaction; r represents an ideal gas constant; t represents a fuel cell operating temperature;
total ohmic loss η of the monolithic fuel cellohmicThe setting is made by the following formula:
ηohmic＝iRohmic
Figure FDA0003131794280000025
wherein R isohmicDenotes the total ohmic resistance, R mRepresents the proton transport resistance of the proton exchange membrane,
Figure FDA0003131794280000026
represents the effective proton transport resistance, R, of the cathode catalyst layerctRepresents the contact resistance between the bipolar plate and the gas diffusion layer;
total concentration loss η of the monolithic fuel cellconThe setting is made by the following formula:
Figure FDA0003131794280000027
wherein, BcDenotes the concentration constant, i, of the cathodelimIndicating the limiting current density.
4. The aging quantification method for a proton exchange membrane fuel cell component as claimed in claim 1, wherein the step 3) is specifically:
the fuel cell mainly comprises a catalytic layer, a proton exchange membrane, a bipolar plate and a gas diffusion layer;
s1: respectively calculating the activation loss and the penetration loss according to the sum of the activation loss and the penetration loss, wherein the activation loss is completely caused by a catalyst layer of the fuel cell, and the penetration loss is completely caused by a proton exchange membrane of the fuel cell;
wherein the activation loss and the permeation loss of the monolithic fuel cell are calculated by the following formulas:
Figure FDA0003131794280000028
Figure FDA0003131794280000029
wherein eta isactRepresents the activation loss, η, of a monolithic fuel cellcrossRepresents the permeation loss of a monolithic fuel cell; i.e. icrossIndicating infiltrationThe current transmission density; i represents a rated load current density; etaact+crossRepresents the sum of the activation loss and the permeation loss of the monolithic fuel cell;
S2: the total ohmic loss is respectively caused by a proton exchange membrane, a catalytic layer and a bipolar plate of the fuel cell, and according to the total ohmic loss, the proton transmission resistance of the proton exchange membrane, the effective proton transmission resistance of the cathode catalytic layer and the contact resistance between the bipolar plate and the gas diffusion layer are respectively calculated by using a transmission line model, so that the ohmic loss caused by the proton exchange membrane, the ohmic loss caused by the catalytic layer and the ohmic loss caused by the bipolar plate are calculated;
wherein the proton transfer resistance R of the proton exchange membrane of the single-chip fuel cellmThe calculation formula is as follows:
Figure FDA0003131794280000031
wherein, deltam,dryThe thickness of the dry proton exchange membrane is expressed,
Figure FDA0003131794280000032
represents the effective proton conductivity, δ, of the proton exchange membraneswellThe expansion ratio of the proton exchange membrane after absorbing water is expressed;
effective proton transport resistance of cathode catalyst layer of monolithic fuel cell
Figure FDA0003131794280000033
The calculation formula of (2) is as follows:
Figure FDA0003131794280000034
wherein the content of the first and second substances,
Figure FDA00031317942800000316
is the proton transport resistance of the catalytic layer, and the constant 3 represents the reaction of protons and oxygen at the interface of the catalytic layer and the gas diffusion layer, ζIs a correction factor that takes into account the effects of oxygen transport limitations;
contact resistance R between bipolar plate and gas diffusion layer of monolithic fuel cellctThe calculation method of (2) is as follows:
Figure FDA0003131794280000035
s3: the total concentration loss is caused by a gas diffusion layer and a catalyst layer of the fuel cell, and according to the total concentration loss of the fuel cell, the average liquid water saturation of the gas diffusion layer and the average liquid water saturation of the catalyst layer are reversely calculated by using a transmission line model to obtain the oxygen transmission resistance of the gas diffusion layer and the catalyst layer, so that the concentration loss caused by the gas diffusion layer and the catalyst layer respectively is obtained;
Wherein the oxygen transmission resistances of the gas diffusion layer and the catalytic layer of the monolithic fuel cell are set by the following formula:
Figure FDA0003131794280000036
wherein, the first and the second end of the pipe are connected with each other,
Figure FDA0003131794280000037
represents the total resistance to oxygen transport of the cathode of a monolithic fuel cell,
Figure FDA0003131794280000038
which represents the resistance to oxygen transport in the monolithic fuel cell cathode flow channel to gas diffusion layer interface,
Figure FDA0003131794280000039
representing the resistance to oxygen transport in the gas diffusion layer of the cathode of the monolithic fuel cell,
Figure FDA00031317942800000310
which represents the resistance to oxygen transport in the cathode catalytic layer of a monolithic fuel cell,
Figure FDA00031317942800000311
represents the local resistance of oxygen transmission in the cathode catalytic layer of the single fuel cell;
Figure FDA00031317942800000312
the resistance to oxygen transmission caused by the gas diffusion layer,
Figure FDA00031317942800000313
oxygen transport resistance due to the catalytic layer;
the concentration losses caused by the gas diffusion layer and the catalytic layer, respectively, are set by the following equations:
Figure FDA00031317942800000314
Figure FDA00031317942800000315
wherein eta iscon1Concentration loss, η, caused by gas diffusion layerscon2Concentration losses caused for the catalytic layer;
s4: and calculating the voltage loss caused by each component of the fuel cell in different aging stages according to the activation loss, the penetration loss, the ohmic loss and the concentration loss caused by each component in the steps S1-S3, wherein the voltage loss caused by the proton exchange membrane is the sum of the penetration loss of the fuel cell and the ohmic loss of the proton exchange membrane, the voltage loss caused by the catalytic layer is the sum of the activation loss of the fuel cell, the ohmic loss of the catalytic layer and the concentration loss of the catalytic layer, the voltage loss caused by the gas diffusion layer is the concentration loss of the gas diffusion layer, and the voltage loss caused by the bipolar plate is the ohmic loss of the bipolar plate.
5. The method of claim 1, wherein the total voltage polarization loss is the sum of activation loss, permeation loss, total ohmic loss, and total concentration loss.
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