CN105789660A - Method and device for detecting consistency of proton exchange membrane fuel cell stack - Google Patents
Method and device for detecting consistency of proton exchange membrane fuel cell stack Download PDFInfo
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Abstract
The invention discloses a method for detecting fluid distribution consistency of a proton exchange membrane fuel cell stack. The proton exchange membrane fuel cell stack consists of over two single cells which are stacked in sequence, and comprises a positive electrode inlet and a negative electrode inlet, wherein mixed gas of hydrogen and inertial gas is introduced into the positive electrode inlet or the negative electrode inlet of the proton exchange membrane fuel cell stack; a voltage for oxidizing hydrogen is applied between the two electrodes of the single cells of the proton exchange membrane fuel cell stack; and the fluid distribution consistency of the proton exchange membrane fuel cell stack is judged in a way of testing and comparing consistency of oxidation current I<n> of the single cells. Compared with the prior art, the method for detecting the fluid distribution consistency of a proton exchange membrane fuel cell and the consistency of the stack is simple and easy to implement; the detection device is simple and easy to assemble; and the method and the device have great significance to accurate detection of the single cell performance of the proton exchange membrane fuel cell stack.
Description
Technical field
The invention belongs to fuel cell field, being specifically related in a kind of fuel cell pile fluid distributes conforming method of testing.
Background technology
Proton Exchange Membrane Fuel Cells is a kind of energy conversion device that fuel chemical energy is converted directly into electric energy, has a generating efficiency height, the advantage such as environmentally friendly, has wide practical use in power, portable and stand-by power supply field.
Pile is fuel cell " heart ", is the place that occurs of electrochemical reaction, in order to being electric energy by the chemical energy of fuel.One pile is made up of to hundreds of joint monocells tens of, and monocell is made up of membrane electrode and the pole plate with runner being positioned at membrane electrode both sides.Monocell performance is inconsistent will affect the performance of Performance data, and shorten service life.
Generation pile discordance mainly has the reason of two aspects: the 1) discordance of membrane electrode, in manufacturing membrane electrode process, technique and uniform in material sex chromosome mosaicism and the performance difference caused；2) discordance of fluid distribution, owing to the pole plate course of processing and pile assembling process cause the resistance drop difference in flow field, causes that the reactant flow entering each monocell is inconsistent, thus causing the performance difference of monocell.
At present satisfactory method is rarely had for the conforming detection of pile.We can detect and often save single battery voltage in running in pile, but this voltage differences is to cause due to the performance difference of membrane electrode own or owing to (reactant flow is inconsistent) under feeding causes, this is difficult to judge.Patent CN102981124A proposes one and judges the conforming method of membrane electrode in pile with electrochemical active surface, but battery performance is still undistinct so far with the relation of electrochemical active surface, the decline of electrochemical active surface not necessarily causes the decline of battery performance, so method is only that pile consistency detection is had some reference value.
For problem above, the present invention provides fluid in the test fuel cell of a kind of simplicity to distribute conforming detection method.Negative electrode (or anode) at fuel cell passes into H2With the gaseous mixture of noble gas, and apply a positive voltage at negative electrode (or anode) and (be enough to H2Complete oxidation), the height of reactant flow in the big I reaction stream road of institute's oxygen determination galvanic current.During test, H2There is electrochemical oxidation at negative electrode (or anode), generate proton and arrive, by ion exchange membrane, the electron reaction generation H that anode (or negative electrode) comes with external circuit2.Due to H2Electrochemical oxidation speed on the catalyst based surface of Pt is very fast, and this reaction is subject to mass transport limitation, the i.e. same H of oxidation current size2Mass transfer flux is correlated with, and H2Mass transfer flux be that the flow with gaseous mixture is closely coupled.Therefore the height of the big I reaction gas flow of oxidation current.
Summary of the invention
For problem above, present invention aim at providing a kind of simple and easy to do conforming method of detection pile.
For achieving the above object, the technical solution used in the present invention is: the conforming detection method of proton exchange film fuel cell electric piling, described proton exchange film fuel cell electric piling by 2 joints above stack gradually and the monocell of gas circuit series connection forms；Described proton exchange film fuel cell electric piling includes an anode inlet and a cathode inlet；
The hydrogen gaseous mixture with noble gas is passed in described proton exchange film fuel cell electric piling anode inlet or cathode inlet, and apply the same voltage for oxidation of hydrogen at proton exchange film fuel cell electric piling each monocell two interpolar, by testing and respectively save the oxidation current I of monocellnConcordance judge the concordance that proton exchange film fuel cell electric piling fluid distributes.
Its theoretical foundation is: H2There is electrochemical oxidation at negative electrode (or anode), generate proton and arrive, by ion exchange membrane, the electron reaction generation H that anode (or negative electrode) comes with external circuit2.Due to H2Electrochemical oxidation speed on the catalyst based surface of Pt base or Pd is very fast, and this reaction is subject to mass transport limitation, the i.e. same H of oxidation current size2Mass transfer flux is correlated with, and H2Mass transfer flux be that the flow with gaseous mixture is closely coupled.Therefore the height of the big I reaction gas flow of oxidation current.
The described voltage being used for oxidation of hydrogen in proton exchange film fuel cell electric piling each monocell two interpolar applying one is specially when passing into the hydrogen gaseous mixture with noble gas in fuel cell pile anode inlet, applies an identical positive voltage at proton exchange film fuel cell electric piling each monocell anode；
Or pass into the hydrogen gaseous mixture with noble gas in proton exchange film fuel cell electric piling cathode inlet, and apply an identical positive voltage at proton exchange film fuel cell electric piling each monocell negative electrode；
The concordance of the oxidation current by testing and respectively saving monocell judges the concordance that fuel cell pile fluid distributes；If described oxidation current is unanimously, enters each cell fluid flow in described pile consistent, if described oxidation current is inconsistent, enter each cell fluid flow in described pile inconsistent.
Optimal conditions in described detection process be proton exchange film fuel cell electric piling respectively save the membrane electrode in monocell stand intact；Optimal conditions is that the membrane electrode performance that proton exchange film fuel cell electric piling respectively saves in monocell is consistent.
The described voltage for oxidation of hydrogen is 0.3-0.9V.
Described positive voltage is 0.3-0.9V.
In described gaseous mixture, the volumetric concentration of hydrogen is 0.1-10%.
Described noble gas is one or more the mixture in nitrogen, helium, argon.
Described monocell includes a membrane electrode and is placed in plate and the cathode plate of its both sides；Described membrane electrode includes a dielectric film and is attached to the eelctro-catalyst of its two side surface；Described eelctro-catalyst is Pt base or Pd base eelctro-catalyst.
The conforming detection method of proton exchange film fuel cell electric piling, described proton exchange film fuel cell electric piling by 2 joints above stack gradually and the monocell of gas circuit series connection forms；Described proton exchange film fuel cell electric piling includes an anode inlet and a cathode inlet；
Described detection method comprises the steps,
(1) each single battery voltage V in fuel cell pile work process is measuredn；
(2) pass into the hydrogen gaseous mixture with noble gas in described fuel cell pile anode inlet or cathode inlet, and apply the voltage being used for oxidation of hydrogen at fuel cell pile each monocell two interpolar, test the oxidation current I of each joint monocelln, find out less than the monocell K corresponding to each joint monocell average oxidation electric current simultaneously, and calculate oxidation current InCorresponding gas flow Qn；
(3) Theoretical Calculation determines that qualified membrane electrode is in operating conditions when gas flow is QnTime corresponding voltage range Vn o；
(4) contrast VnAnd Vn oIf, VnAt Vn oWithin scope, then monocell K performance difference come from pile fluid distribution inconsistent, if VnLess than Vn o, then monocell K performance difference is also relevant to membrane electrode itself.
Described step (2) test process is specially and passes into the hydrogen gaseous mixture with noble gas in proton exchange film fuel cell electric piling anode inlet, and applies an identical positive voltage between proton exchange film fuel cell electric piling each monocell anode；Or pass into the hydrogen gaseous mixture with noble gas in proton exchange film fuel cell electric piling cathode inlet, and between proton exchange film fuel cell electric piling each monocell negative electrode, apply an identical positive voltage.
The described voltage for oxidation of hydrogen is 0.3-0.9V.
The positive voltage of described applying is 0.3-0.9V.
In described gaseous mixture, the volumetric concentration of hydrogen is 0.1-10%.
Described noble gas is one or more the mixture in nitrogen, helium, argon.
Described monocell includes a membrane electrode and is placed in plate and the cathode plate of its both sides；Described membrane electrode includes a dielectric film and eelctro-catalyst attached to it；Described eelctro-catalyst be Pt base or Pd catalyst based.
The concrete testing procedure of the conforming detection method of a kind of proton exchange film fuel cell electric piling is:
(1) H is passed into negative electrode (or anode) chamber of fuel cell pile2Gaseous mixture with noble gas；
Described noble gas is N2, one or more in Ar, He；
In described gaseous mixture, the concentration of hydrogen is 0.1-10%；
Described gaseous mixture can be humidified and can not also be humidified；
The used catalyst of described Proton Exchange Membrane Fuel Cells is that Pt or Pd is catalyst based.
(2) negative electrode (or anode) of each monocell is applied a positive potential, as shown in Figure 3,4, record current size；
Described positive potential be sized to 0.3-0.9V；
Another chamber of described test pile can pass into noble gas (N2, one or more in Ar, He) or deionized water, also can be obstructed.
(3) flow ratio, i.e. i in each monocell of entrance is drawn according to test size of current1: i2: i3: ... in=Q1: Q2: Q3:…Qn；
I in formulanIt is the n-th joint monocell test current value, QnFor entering the n-th joint monocell gas flow.Know total gas flow rate in entrance pile, just can calculate, according to above formula, the gas flow entered in each monocell.
Principles of the invention is set forth below in conjunction with Fig. 1 and Fig. 2.Fig. 1 is monocell schematic diagram, wherein 1 PEM；2 and 2 ' is Catalytic Layer；3 and 3 ' is diffusion layer；4 and 4 ' is the pole plate with runner.During test, the negative electrode 4 ' (or anode) at fuel cell passes into H2And N2Gaseous mixture, applies a positive potential at negative electrode (or anode), now H afterwards2In Catalytic Layer 2 ', electroxidation occurring, the proton of generation arrives Catalytic Layer 2 by PEM 1, and the electronics generation electro-reduction reaction come with external circuit at Catalytic Layer 2 proton generates H2.The electric current arrived detected calculates by formula (1),
I=J × nF (1)
In formula (1), i is electric current, and J is hydrogen molar flux, and F is Faraday constant, and n is number of electron exchange, here for 2.Mass transfer flux J is relevant to entering gas flow Q in battery, illustrates with Fig. 2 below.Fig. 2 is H in test process2CONCENTRATION DISTRIBUTION schematic diagram, in figure, 2 is Catalytic Layer；3 is diffusion layer；4 is the pole plate with runner.Under steady state conditions
J=k (Cch-Ccl)(2)
Wherein, CchFor H in runner2Concentration, CclFor H in Catalytic Layer2Concentration, k mass tranfer coefficient.Sufficiently high because applying current potential, hydrogen is fully oxidized, i.e. H in Catalytic Layer2Concentration Ccl=0, therefore know that mass transfer flux J is directly proportional with mass tranfer coefficient from formula 2, know mass transfer correlation according to dimensional analysis,
K=f (Re, Sc) (3)
Wherein, Re is Reynolds number, and Sc is Schmidt number (only relevant to physical properties of fluids, to be a constant in this experiment).It can be seen that k and Reynolds number are closely related, and
Re=dv ρ/μ ∝ Q (4)
Wherein, d is runner hydraulic diameter, and v is flow velocity, and ρ is density, and μ is viscosity.After fluid is determined, Re only becomes with flow velocity v, and flow velocity is directly proportional with flow, therefore Re is directly proportional with fluid flow Q.The known electric current i in composite type (1)-(4) is closely related with fluid flow Q, therefore can reflect by size of current and enter the uninterrupted of fluid in runner.Being found through experiments in conventional gas flow scope, namely generally at the measurement of gas flow ratio during lower than 5, electric current is linear relationship (as shown in Figure 5) with flow, namely
i∝Q(5)
Now the n-th joint monocell QnGas flow be assigned as and can be calculated by equation below
M represents that in pile, m saves monocell, imIt is that m saves monocell test current value, QmMonocell gas flow is saved for entering m.
M, n are the positive integer of > 2.
Certain electric current is not limited to above linear relationship with discharge relation.
A kind of proton exchange film fuel cell electric piling fluid distributes conforming detection method detection device thereof, including mixed gas supply device, DC source and current detection module；
Described mixed gas supply device is for providing gaseous mixture for proton exchange film fuel cell electric piling anode inlet or cathode inlet；Described DC source and current detection module are for applying voltage for each monocell of proton exchange film fuel cell electric piling and detecting the electric current of each monocell of proton exchange film fuel cell electric piling simultaneously.
Described power supply and current detection module can integrated device, also can be separate supply unit and current sensing means.
It is electrochemical workstation or programmable power supply when described power supply and the integrated device of current detection module.
When described power supply and current detection module are separate supply unit and current sensing means, supply unit is the one in gate-controlled switch power supply, power module, and current sensing means is the one in ammeter, Hall current sensor, current detection module.
Illustrating for Fig. 6, test device possesses: 1. gas flow control device, including valve 601,602,603, mass flowmenter 604,605,606；2 gas mixers 610；3 insulating power supplies 650, data acquisition and processing unit 640.
Described insulating power supply be multiple can independently to pile execute alive power supply composition, described insulating power supply can be multiple constant pressure sources measuring function with belt current, as it is shown in fig. 7, described constant pressure source can be the one in electrochemical workstation, programmable power supply, Switching Power Supply.
Described insulating power supply is standalone module power supply and detection current device composition, as shown in Figure 8, it is possible to be the one in ammeter, Hall current sensor, current detection module.
Compared with prior art, detection Proton Exchange Membrane Fuel Cells fluid of the present invention distribution concordance and the conforming detection method of pile, simply being easily achieved, detecting device is simply easily assembled to, significant for accurately detecting proton exchange film fuel cell electric piling each monocell performance.
Accompanying drawing explanation
Fig. 1 is the schematic diagram of Proton Exchange Membrane Fuel Cells monocell.
Wherein, 1 PEM；2 and 2 ' respectively the first and second Catalytic Layer；3 and 3 ' respectively the first and second diffusion layers；4 and 4 ' respectively with the first and second pole plates of runner.
Fig. 2 is H in membrane electrode in test process2CONCENTRATION DISTRIBUTION schematic diagram, wherein 2 is Catalytic Layer；3 is diffusion layer；4 is the pole plate with runner.
Fig. 3 is pile test schematic diagram, passes into H in pile cathode chamber2、N2Gaseous mixture, now need to apply a positive potential at the negative electrode of monocell.
Fig. 4 is pile test schematic diagram, passes into H in pile anode chamber2、N2Gaseous mixture, now need to apply a positive potential at the anode of monocell.
When Fig. 5 is different membrane electrode decrement, test electric current is with the relation of gas flow.
Fig. 6 is the schematic diagram of detecting device.Wherein 601,602,603 is valve, and 604,605,606 is mass flowmenter, and 610 is blender, and 620 is fuel cell pile, and 640 is data acquisition and processing unit, and 650 is power supply.
Fig. 7 is insulating power supply 650 schematic diagram, the constant pressure source that wherein 701,702,703,704,705,706 is belt current measurement function, it is possible to be the one in electrochemical workstation, programmable power supply, Switching Power Supply.
Fig. 8 is insulating power supply 650 schematic diagram, wherein 801,802,803,804,805,806 is modular power source, 811,812,813,814,815,816 is detection current device, it is possible to be the one in ammeter, Hall current sensor, sample resistance and high side current detection amplifier.
Detailed description of the invention
Below in conjunction with embodiment, the present invention is explained in detail.Certain present invention is not limited in following specific embodiment.
Embodiment 1
Pile used contains three joint monocells.Monocell area is 25cm2, PEM used is Nafion115, and catalyst is Pt/C.H is passed into negative electrode during test2And N2Gaseous mixture, total flow is 1L/min, H2Volumetric concentration is 1.5%, and anode chamber does not pass into any fluid but keeps and atmosphere.Use electrochemical workstation Soltron1287 that each monocell negative electrode is applied a 0.6V positive potential, record current size afterwards.Fig. 3 is shown in by test schematic diagram, and test result is as follows:
| Battery is numbered | Size of current mA |
| 1 | 517.4 |
| 2 | 446.4 |
| 3 | 494.3 |
Embodiment 2
Pile used contains three joint monocells.Monocell area is 25cm2, PEM used is Nafion115, and catalyst is Pt/C.H is passed into anode chamber during test2And N2Gaseous mixture, H2Volumetric concentration is 1.5%, and cathode chamber passes into deionized water.Use DC source safe and sound letter PPS3005 that each monocell negative electrode is applied a 0.9V positive potential, record current size afterwards.Fig. 4 is shown in by test schematic diagram, and test result is as follows:
| Battery is numbered | Size of current mA |
| 1 | 561.2 |
| 2 | 376.4 |
| 3 | 525.6 |
Embodiment 3
Pile used contains six joint monocells.Monocell area is 25cm2, PEM used is Nafion212, and catalyst is Pt/C.Pass into the H of saturated humidification to cathode chamber during test2、N2Gaseous mixture, total flow is 1L/min, H2Volumetric concentration is 2%, and anode chamber passes into saturated humidification N2.Use isolation module power supply as shown in Figure 8 that each monocell negative electrode is applied a 0.8V positive potential, record current size afterwards.Testing hydrogen-air fuel cell performance in 65 DEG C of saturated humidification situations afterwards, be 7.5L/min in air mass flow, record is at 1A/cm2Each unit voltage in constant-current discharge situation.For hydrogen-air fuel cell, anode side hydrogen pneumoelectric oxidation rate is exceedingly fast, and the overpotential of battery is mainly caused by the mass transfer reaction process of negative electrode oxygen.Therefore to using H2Do the difference of the Proton Exchange Membrane Fuel Cells main cathode performance of fuel.Test and result of calculation are shown in following table.
Therefrom find out battery 3,4 low voltage.Known for battery 4 by analysis, its Vn<Vn o, then the own slightly inferior properties of its membrane electrode.And for battery 3, its VnValue drops within the scope of qualified voltage, then the reason that its voltage is low is in that amount of supplied air is on the low side.
Claims (19)
1. the conforming detection method of proton exchange film fuel cell electric piling, it is characterised in that: proton exchange film fuel cell electric piling by 2 joints above stack gradually and the monocell of gas circuit series connection forms；Described proton exchange film fuel cell electric piling includes an anode inlet and a cathode inlet；
The hydrogen gaseous mixture with noble gas is passed in described proton exchange film fuel cell electric piling anode inlet or cathode inlet, and apply the same voltage for oxidation of hydrogen at proton exchange film fuel cell electric piling each monocell two interpolar, by testing and respectively save the oxidation current I of monocellnConcordance judge the concordance that proton exchange film fuel cell electric piling fluid distributes.
2. detection method as claimed in claim 1, it is characterized in that: the described voltage being used for oxidation of hydrogen in proton exchange film fuel cell electric piling each monocell two interpolar applying one is specially when passing into the hydrogen gaseous mixture with noble gas in fuel cell pile anode inlet, applies an identical positive voltage at proton exchange film fuel cell electric piling each monocell anode；
Or pass into the hydrogen gaseous mixture with noble gas in proton exchange film fuel cell electric piling cathode inlet, and apply an identical positive voltage at proton exchange film fuel cell electric piling each monocell negative electrode；
The concordance of the oxidation current by testing and respectively saving monocell judges the concordance that fuel cell pile fluid distributes；If described oxidation current is unanimously, enters each cell fluid flow in described pile consistent, if described oxidation current is inconsistent, enter each cell fluid flow in described pile inconsistent.
3. the detection method as described in as arbitrary in claim 1-2, it is characterised in that: the optimal conditions in described detection process is that proton exchange film fuel cell electric piling respectively saves the membrane electrode in monocell and stands intact；Optimal conditions is that the membrane electrode performance that proton exchange film fuel cell electric piling respectively saves in monocell is consistent.
4. detection method as claimed in claim 1, it is characterised in that: the described voltage for oxidation of hydrogen is 0.3-0.9V.
5. detection method as claimed in claim 2, it is characterised in that: described positive voltage is 0.3-0.9V.
6. the detection method as described in as arbitrary in claim 1-2, it is characterised in that: in described gaseous mixture, the volumetric concentration of hydrogen is 0.1-10%.
7. the detection method as described in as arbitrary in claim 1-2, it is characterised in that: described noble gas is one or more the mixture in nitrogen, helium, argon.
8. detection method as claimed in claim 1, it is characterised in that: described monocell includes a membrane electrode and is placed in plate and the cathode plate of its both sides；Described membrane electrode includes a dielectric film and is attached to the eelctro-catalyst of its two side surface；Described eelctro-catalyst is Pt base or Pd base eelctro-catalyst.
9. the conforming detection method of proton exchange film fuel cell electric piling, it is characterised in that: a proton exchange film fuel cell electric piling by 2 joints above stack gradually and the monocell of gas circuit series connection forms；Described proton exchange film fuel cell electric piling includes an anode inlet and a cathode inlet；
Described detection method comprises the steps,
(1) each single battery voltage V in fuel cell pile work process is measuredn；
(2) pass into the hydrogen gaseous mixture with noble gas in described fuel cell pile anode inlet or cathode inlet, and apply the voltage being used for oxidation of hydrogen at fuel cell pile each monocell two interpolar, test the oxidation current I of each joint monocelln, find out less than the monocell K corresponding to each joint monocell average oxidation electric current simultaneously, and calculate oxidation current InCorresponding gas flow Qn；
(3) Theoretical Calculation determines that qualified membrane electrode is in operating conditions when gas flow is QnTime corresponding voltage range Vn°；
(4) contrast VnAnd Vn°, if VnAt VnWithin ° scope, then to come from the distribution of pile fluid inconsistent for monocell K performance difference, if VnLess than Vn°, then monocell K performance difference is also relevant to membrane electrode itself.
10. detection method as claimed in claim 9, it is characterized in that: described step (2) test process is specially and passes into the hydrogen gaseous mixture with noble gas in proton exchange film fuel cell electric piling anode inlet, and applies an identical positive voltage between proton exchange film fuel cell electric piling each monocell anode；Or pass into the hydrogen gaseous mixture with noble gas in proton exchange film fuel cell electric piling cathode inlet, and between proton exchange film fuel cell electric piling each monocell negative electrode, apply an identical positive voltage.
11. detection method as claimed in claim 9, it is characterised in that: the described voltage for oxidation of hydrogen is 0.3-0.9V.
12. detection method as claimed in claim 10, it is characterised in that: the positive voltage of described applying is 0.3-0.9V.
13. the detection method as described in as arbitrary in claim 9-10, it is characterised in that: in described gaseous mixture, the volumetric concentration of hydrogen is 0.1-10%.
14. the detection method as described in as arbitrary in claim 9-10, it is characterised in that: described noble gas is one or more the mixture in nitrogen, helium, argon.
15. detection method as claimed in claim 9, it is characterised in that: described monocell includes a membrane electrode and is placed in plate and the cathode plate of its both sides；Described membrane electrode includes a dielectric film and eelctro-catalyst attached to it；Described eelctro-catalyst be Pt base or Pd catalyst based.
16. the arbitrary described proton exchange film fuel cell electric piling fluid of claim 1-15 distributes conforming detection method detection device thereof, it is characterised in that: include mixed gas supply device, DC source and current detection module；
Described mixed gas supply device is for providing gaseous mixture for proton exchange film fuel cell electric piling anode inlet or cathode inlet；Described DC source and current detection module are for applying voltage for each monocell of proton exchange film fuel cell electric piling and detecting the electric current of each monocell of proton exchange film fuel cell electric piling simultaneously.
17. as claimed in claim 16 detecting device, it is characterised in that: described power supply and current detection module can integrated device, also can be separate supply unit and current sensing means.
18. as claimed in claim 16 detecting device, it is characterised in that: it is electrochemical workstation or programmable power supply when described power supply and the integrated device of current detection module.
19. detecting device as claimed in claim 16, it is characterized in that: when described power supply and current detection module are separate supply unit and current sensing means, supply unit is the one in gate-controlled switch power supply, power module, and current sensing means is the one in ammeter, Hall current sensor, current detection module.
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| PCT/CN2014/094472 WO2016095238A1 (en) | 2014-12-15 | 2014-12-22 | Method and device for detecting pile consistency of proton exchange membrane fuel cell |
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| WO2016095238A1 (en) | 2016-06-23 |
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