CN108232258B - Methanol-dimethyl ether mixed steam feeding fuel cell system - Google Patents

Methanol-dimethyl ether mixed steam feeding fuel cell system Download PDF

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CN108232258B
CN108232258B CN201611156982.9A CN201611156982A CN108232258B CN 108232258 B CN108232258 B CN 108232258B CN 201611156982 A CN201611156982 A CN 201611156982A CN 108232258 B CN108232258 B CN 108232258B
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fuel cell
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methanol
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CN108232258A (en
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杨林林
孙公权
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Dalian Institute of Chemical Physics of CAS
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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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
    • H01M8/1011—Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
    • 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
    • H01M8/04007—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids related to heat exchange
    • H01M8/04014—Heat exchange using gaseous fluids; Heat exchange by combustion of reactants
    • 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
    • H01M8/04007—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids related to heat exchange
    • H01M8/04014—Heat exchange using gaseous fluids; Heat exchange by combustion of reactants
    • H01M8/04022—Heating by combustion
    • 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
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • 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 provides a methanol-dimethyl ether mixed steam feeding fuel cell system, which comprises a mixed fuel storage tank, a fuel cell single battery or a fuel cell stack and an air pump, wherein the mixed fuel storage tank is arranged in the fuel cell system; the mixed fuel storage tank stores mixed fuel of methanol and dimethyl ether, and the mole fraction of the methanol in the mixed fuel is 5-40%; the outlet of the mixed fuel storage tank is communicated with the anode inlet of the single fuel cell or the fuel cell stack to provide reaction fuel for the anode of the single fuel cell or the fuel cell stack; the air pump provides oxidant for the fuel cell or fuel cell stack cathode. Compared with the prior art, the methanol-dimethyl ether mixed gas phase separation system has the advantages that the methanol and the dimethyl ether are mixed in a certain proportion, so that gaseous feeding under the condition of no need of an external vaporizer can be realized, and the system structure is greatly simplified; meanwhile, the fuel permeation is greatly reduced, and the performance of the battery is improved.

Description

Methanol-dimethyl ether mixed steam feeding fuel cell system
Technical Field
The invention belongs to the field of fuel cells, and particularly relates to a methanol-dimethyl ether mixed steam feeding fuel cell.
Background
The fuel cell is an energy conversion device for directly converting chemical energy of fuel into electric energy, has the advantages of high efficiency, no pollution, low noise and the like, and has wide application prospect in the fields of power supplies, standby power supplies and mobile power supplies.
The liquid methanol is convenient to store and transport, has higher electrochemical oxidation rate, and is an ideal fuel for the fuel cell. In the field of portable power sources, the Direct Methanol Fuel Cell (DMFC) has obvious advantages and has applications in many aspects such as field exploration, unattended operation and the like. Methanol crossover, however, is a major international problem with DMFC, which leads to three consequences: firstly, the fuel utilization rate is reduced, secondly, the mixed potential is caused to cause voltage drop, thirdly, the flooding is intensified, and the oxygen mass transfer resistance is increased (methanol permeates from the anode to the cathode to react with oxygen to generate water).
In order to alleviate the negative effects of methanol permeation, the following methods are commonly used: 1. an electrolyte membrane with small alcohol-water permeability coefficient is selected, which can reduce proton conductivity or reduce service life; 2. the cathode uses a methanol tolerant catalyst, which simply eliminates the mixing potential.
The liquid water and alcohol have high permeability in the proton exchange membrane Nafion, but the gas methanol has lower permeability in the Nafion membrane by several orders of magnitude. Thus, methanol permeation can be greatly reduced with methanol vapor feed. However, methanol is liquid at normal temperature, a large amount of heat is required for vaporization, and a vaporizer is used in a battery system, which undoubtedly increases the complexity and the volume weight of the system.
Aiming at the problems, the invention provides a fuel cell fed by a methanol-dimethyl ether mixed fuel. Dimethyl ether is a common chemical product, is in a gaseous state at normal temperature, and has liquefaction pressure of only 5 atmospheric pressures. The electric oxidation rate of the dimethyl ether is slower than that of the methanol, so that the performance of the direct dimethyl ether fuel cell is lower than that of the direct methanol fuel cell. If methanol and dimethyl ether are mixed in a certain proportion, gaseous feeding can be realized without an external vaporizer, and the system structure is greatly simplified; meanwhile, the fuel permeation is greatly reduced, and the performance of the battery is improved.
Disclosure of Invention
In view of the above problems, the present invention aims to provide a methanol-dimethyl ether mixed steam feed fuel cell.
In order to achieve the purpose, the invention adopts the technical scheme that:
a methanol-dimethyl ether mixed steam feed fuel cell system comprises a mixed fuel storage tank, a fuel cell single cell or a fuel cell stack and an air pump; the mixed fuel storage tank stores mixed fuel of methanol and dimethyl ether, and the mole fraction of the methanol in the mixed fuel is 5-40%; the outlet of the mixed fuel storage tank is communicated with the anode inlet of the single fuel cell or the fuel cell stack to provide reaction fuel for the anode of the single fuel cell or the fuel cell stack; the air pump provides oxidant for the fuel cell or fuel cell stack cathode.
The mixed fuel storage tank is a pressure storage tank, and a pressure reducing valve is arranged between an outlet of the pressure storage tank and an anode inlet of the fuel cell single battery or the fuel cell stack. The mixed fuel is decompressed by the pressure reducing valve and then enters the anode chamber of the fuel cell stack, and air enters the cathode chamber of the fuel cell by the air pump, as shown in fig. 3.
The single fuel cell has a self-return water electrode structure, that is, water generated by cathode reaction can reach the anode through the proton exchange membrane. The main reaction of the cathode and the anode during the operation of the battery is
Anode: CH (CH)3OH+H20→CO2+6H+
CH3OCH3+3H20→2CO2+12H+
Cathode:
Figure BDA0001180813200000021
from the above formula, it can be seen that the anode reaction requires water, while the cathode generates water, and the amount of generated water is about 2 times the amount of water required. The water generated by the cathode can be supplemented to the anode through the proton exchange membrane by adopting the self-water-return membrane electrode, so that the water balance of the cell is realized.
The chemical potential of water at the cathode side in the self-water-return MEA is far greater than that of water at the anode side, and the chemical potential of water in the porous medium is related to surface tension, activity, gravity and static pressure:
Figure BDA0001180813200000022
the right end of the above formula is respectively a standard chemical potential, a permeability term, a static pressure term, a capillary pressure term and a gravity term. According to the above formula, the self-return of the membrane electrode can be realized by adjusting the materials and structures of the cathode catalyst layer and the diffusion layer to make the chemical potential of the cathode water greater than that of the anode.
The self-returning water electrode means that the chemical potential of water at the cathode side is greater than that at the anode side; the anode side of the self-water-return electrode is hydrophilic, the contact angle of water in the pores of the anode catalyst layer and the microporous layer is between 30 and 80 degrees, the porosity of the anode catalyst layer and the microporous layer is between 20 and 50 percent, and the average pore diameter is between 0.02 and 0.5 micron; the cathode side is hydrophobic, the contact angle of water in pores in the cathode catalyst layer and the microporous layer is between 100 and 150 degrees, the porosity of the cathode catalyst layer and the microporous layer is between 20 and 40 percent, and the average pore diameter is between 0.02 and 0.2 micrometer. 4. The methanol-dimethyl ether mixed vapor feed fuel cell system of claim 1, wherein: the fuel cell system also comprises a gas-liquid separator, wherein the inlet of the gas-liquid separator is communicated with the outlet of the cathode of the single fuel cell or the fuel cell stack and is used for separating water generated by the cathode of the single fuel cell or the fuel cell stack and communicated with the inlet of the anode. The separated water and the mixed fuel enter the catalytic combustion heat exchange chamber together and then enter the anode chamber of the fuel cell, so that the water return load of the self-return membrane electrode can be reduced. As shown in fig. 5.
The fuel cell system also comprises a catalytic combustion chamber and a heat exchange chamber which are attached to each other, the outlet of the anode of the single fuel cell or the fuel cell stack is communicated with the inlet of the catalytic combustion chamber and used for enabling tail gas at the outlet of the anode of the single fuel cell or the fuel cell stack to generate combustion reaction, and heat emitted by the combustion reaction is used for heating mixed fuel which enters the anode of the single fuel cell or the fuel cell stack after passing through the heat exchange chamber, so that the temperature difference of the inlet and the outlet in the stack is reduced, and the service life is prolonged. As shown in fig. 3.
The fuel cell system also comprises a gas-liquid separator, a catalytic combustion chamber and a heat exchange chamber which are mutually attached; the inlet of the gas-liquid separator is communicated with the outlet of the cathode of the single fuel cell or the fuel cell stack and is used for separating water generated by the cathode of the single fuel cell or the fuel cell stack; and the gas outlet of the gas-liquid separator is communicated with the inlet of the catalytic combustion chamber and is used for enabling tail gas at the outlet of the anode of the single fuel cell or the fuel cell stack to generate combustion reaction, and the heat released by the combustion reaction is used for heating mixed fuel which enters the anode of the single fuel cell or the fuel cell stack after passing through the heat exchange chamber.
The proton exchange membrane used by the fuel cell is perfluorosulfonic acid, meta-fluorosulfonic acid, sulfonated hydrocarbon membrane, PBI/H3PO4、CsH2PO4One of (1);
one or more than two of the catalysts PtRu/C, PtRuSn/C, PtRuPd/C of the fuel cell anode;
the fuel cell cathode catalyst is one or more than two alloys of platinum, palladium, ruthenium, nickel, chromium, cobalt, copper, tungsten, iron, cerium and molybdenum, or one or more than two alloys of more than two carbon-supported metals.
Compared with the prior art, the methanol-dimethyl ether mixed gas phase separation system has the advantages that the methanol and the dimethyl ether are mixed in a certain proportion, so that gaseous feeding under the condition of no need of an external vaporizer can be realized, and the system structure is greatly simplified; meanwhile, the fuel permeation is greatly reduced, and the performance of the battery is improved.
Drawings
Fig. 1 is a schematic diagram of a self-return water membrane electrode, where water generated at the cathode permeates to the anode through a proton exchange membrane.
Wherein 101 is an anode plate; 102 is an anode diffusion layer; 103 is an anode microporous layer; 104 is an anode catalytic layer; 105 is a proton exchange membrane; 106 is a cathode catalyst layer; 107 is a cathode microporous layer; 108 is a cathode diffusion layer; and 109, a cathode plate.
Figure 2 shows the performance of a single cell with different fuels.
Fig. 3 is a schematic diagram of a methanol-dimethyl ether fuel cell system.
Wherein 301 is a pressure storage tank for storing the methanol-dimethyl ether mixed fuel; 302 is a fuel cell stack; 303 is an air pump; 304 is a pressure reducing valve.
Fig. 4 is a schematic diagram of a methanol-dimethyl ether fuel cell system.
Wherein 301 is a pressure storage tank for storing the methanol-dimethyl ether mixed fuel; 302 is a fuel cell stack; 303 is an air pump; 304 is a pressure reducing valve; 305 is a catalytic combustion heat exchange chamber.
Fig. 5 is a schematic diagram of a methanol-dimethyl ether fuel cell system.
Wherein 301 is a pressure storage tank for storing the methanol-dimethyl ether mixed fuel; 302 is a fuel cell stack; 303 is an air pump; 305 is a catalytic combustion heat exchange chamber; 306 is a condensate-gas-liquid separator.
Detailed Description
The present invention will be described in detail with reference to examples. Of course, the present invention is not limited to the specific examples described below.
Example 1:
the membrane electrode comprises the following components: the gas diffusion layers of the cathode and the anode are all TGP-060; the anode microporous layer is a mixture of carbon powder and Nafion with the mass fraction of 0.5mg/cm2, wherein the Nafion accounts for 10%; the anode catalyst layer is a PtRuPd/C, Nafion mixture, wherein the mass fraction of Nafion is 15%, the anode microporous layer is a carbon powder and PTFE mixture of 2mg/cm2, wherein the mass fraction of PTFE is 30%; the anode catalytic layer is a Pt/C, Nafion solution mixture, wherein the mass fraction of Nafion is 20%. The proton exchange membrane used was Nafion 212.
The materials of the above formula are arranged in sequence in figure 1, and are hot-pressed for one minute at 120 ℃ under 2000 pounds of pressure to form an integrated membrane electrode. The integrated membrane electrode is manufactured by the stainless steel end plate with the punctiform flow field and is sequentially assembled into a battery.
The mixed solution of methanol and dimethyl ether (20% methanol, 80% dimethyl ether) is introduced into the anode of the fuel cell at a flow rate of 80sccm, 500sccm of air is introduced into the cathode, the performance of the fuel cell is tested at 80 ℃ by adopting an electronic load, and the i-V curve is shown as a short horizontal line in FIG. 2.
Comparative example 1: the cell was the same as in example 1, using 1M methanol as the fuel at a flow rate of 1mL/min, 500sccm of air was introduced into the cathode, and the performance was tested at 80 ℃ using an electronic load, and the i-V curve is shown as the solid line in FIG. 2.
Comparative example 2: the cell was the same as in example 1, the fuel used was dimethyl ether at a flow rate of 80sccm, 500sccm of air was introduced into the cathode, and the performance was tested at 80 ℃ using an electronic load, the i-V curve being shown in dotted line in fig. 2.
Example 2:
the membrane electrode comprises the following components: the gas diffusion layers of the cathode and the anode are all TGP-060; the anode microporous layer is a mixture of carbon powder and Nafion with the mass fraction of 0.5mg/cm2, wherein the Nafion accounts for 10%; the anode catalytic layer is a PtRuSn/C, Nafion mixture, wherein the mass fraction of Nafion is 15%, and the anode microporous layer is 2mg/cm2The carbon powder and the PTFE mixture, wherein the mass fraction of the PTFE is 30 percent; the anode catalytic layer is a Pt/C, Nafion solution mixture, wherein the mass fraction of Nafion is 20%. The proton exchange membrane used was Nafion 212. In order to improve the water return capacity of the cathode, a water resisting layer is added between the cathode diffusion layer and the polar plate, the water resisting layer mainly comprises a mixture of carbon powder and PTFE, and the loading capacity is 0.8mg/cm2. The above materials are hot pressed at 120 deg.C under 2000 pounds pressure for one minuteAnd (4) an integrated membrane electrode. The integrated membrane electrode is manufactured by the stainless steel end plate with the punctiform flow field and is sequentially assembled into a battery.
The battery is at 100mA/cm2The voltages are shown in the table below, and the performance is clearly superior at high current densities compared to example 1.
Example 1 Example 2
100mA/cm2 0.591 0.595
200mA/cm2 0.532 0.548

Claims (3)

1. A methanol-dimethyl ether mixed steam feed fuel cell system is characterized in that: the fuel cell system comprises a mixed fuel storage tank, a fuel cell single battery or a fuel cell stack and an air pump; the mixed fuel storage tank stores mixed fuel of methanol and dimethyl ether, and the mole fraction of the methanol in the mixed fuel is 5-40%; the outlet of the mixed fuel storage tank is communicated with the anode inlet of the single fuel cell or the fuel cell stack to provide reaction fuel for the anode of the single fuel cell or the fuel cell stack; the air pump provides an oxidant for the cathode of the fuel cell single cell or the fuel cell stack, the fuel cell single cell has a self-water-returning electrode structure, and the chemical potential of water at the cathode side is greater than that at the anode side; the anode side of the self-water-return electrode is hydrophilic, the contact angle of water in the pores of the anode catalyst layer and the microporous layer is between 30 and 80 degrees, the porosity of the anode catalyst layer and the microporous layer is between 20 and 50 percent, and the average pore diameter is between 0.02 and 0.5 micrometer; the cathode side is hydrophobic, the contact angle of water in pores in the cathode catalyst layer and the microporous layer is between 100 and 150 degrees, the porosity of the cathode catalyst layer and the microporous layer is between 20 and 40 percent, and the average pore diameter is between 0.02 and 0.2 micrometer; the fuel cell system also comprises a gas-liquid separator, a catalytic combustion chamber and a heat exchange chamber which are mutually attached; the inlet of the gas-liquid separator is communicated with the outlet of the cathode of the single fuel cell or the fuel cell stack and is used for separating water generated by the cathode of the single fuel cell or the fuel cell stack; the gas outlet of the gas-liquid separator is communicated with the inlet of the catalytic combustion chamber and is used for enabling tail gas at the outlet of the anode of the single fuel cell or the fuel cell stack to generate combustion reaction, and heat released by the combustion reaction is used for heating mixed fuel which enters the anode of the single fuel cell or the fuel cell stack after passing through the heat exchange chamber;
the mixed fuel storage tank is a pressure storage tank, a pressure reducing valve is arranged between an outlet of the pressure storage tank and an anode inlet of the single fuel cell or the fuel cell stack, and the methanol is mixed with the dimethyl ether, so that gaseous feeding under the condition of not needing an external vaporizer is realized.
2. The methanol-dimethyl ether mixed vapor feed fuel cell system of claim 1, wherein: the proton exchange membrane used by the fuel cell is one of perfluorosulfonic acid, meta-fluorosulfonic acid, sulfonated hydrocarbon membrane, PBI/H3PO4 and CsH2PO 4.
3. The methanol-dimethyl ether mixed vapor feed fuel cell system of claim 1, wherein: one or more than two of the catalysts PtRu/C, PtRuSn/C, PtRuPd/C of the fuel cell anode; the fuel cell cathode catalyst is one or more than two alloy of platinum, palladium, ruthenium, nickel, chromium, cobalt, copper, tungsten, iron, cerium and molybdenum.
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US20040247960A1 (en) * 2003-03-31 2004-12-09 Kabushiki Kaisha Toshiba Fuel cell system
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