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`Primary document | PA3
`*
`*
`NOTICE
`
`:
`
`JPO and INPIT are not responsible for any damages caused by the use of this
`translation.
`
`1. This document has been translated by computer. So the translation may not reflect
`the original precisely.
`****
`shows a word which cannot be translated.
`2.
`3. In the drawings, any words are not translated.
`
`
`
`A
`
`(19) [Publication country] JP
`(12) [Kind of official gazette]
`(11) [Publication number] 05021079
`(43) [Date of publication of application] 19930129
`(54) [Title of the invention] HYDROGEN PRESSURE RAISING DEVICE AND FUEL C
`ELL USING THIS
`
`(51) [International Patent Classification 5th Edition]
`HO1M 8/04
`HOiM 8/06
`HOQ1M 8/10
`
`https://www j-platpat.inpit.¢o.jp/p0200
`
`2021/04/12
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`

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`Patent/Utility Model Document Display | J-PlatPat [JPP]
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`Page 2 of 12
`
`(21) [Application number] 03171141
`(22) [Filing date] 19910711
`
`(71) [Applicant]
`[Name] MITSUBISHI HEAVY IND LTD
`
`(72) [Inventor]
`[Full name] FURUYA CHOICHI
`[Full name} ICHIKAWA KUNINOBU
`[Full name] WADA KO
`[Full name] MINEO TOKUICHI
`
`
`
`a
`
`a
`
`(57) [Overview]
`hydrogen pressure rise device for taking
`PURPOSE: To provide
`high pressure
`hydrogen gas from a low pressure hydrogen gas, and to raise output density of a
`fuel cell using this device.
`CONSTITUTION: A solid high polymer electrolytic film 101 is sandwiched between
`are connected toget
`respective gas diffusion electrodes 102A and 102B, and they
`her, while a power source 107 is connected to the gas diffusion electrodes 102A,
`to a
`102B. When a
`hydrogen including gas is supplied
`hydrogen supply groove 10
`5a of a gas separator 105 in the side of the gas diffusion electrode 102 connected
`a
`to a
`hydrogen gas of high pressure is taken from a
`positive electrode,
`hydrogen
`discharge groove 106a of a gas separator 106 in the side of the gas diffusion elec
`trode 102B connected to a negative electrode. When the hydrogen gas thus obtai
`to a
`hydrogen pole of a fuel cell, the output density is improved.
`ned is supplied
`
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`Page
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`107
`
` LOO sKEFERe
`
`L105, 106 WAL -Y
`
`io? im
`
`
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`https://www j-platpat.inpit.¢o.jp/p0200
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`2021/04/12
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`101 HemeTeaR
`
`102A, 1028 ARH
`
`103A, 103B Riek
`
`LO4A, 104B
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`Patent/Utility Model Document Display | J-PlatPat [JPP]
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`Page 4 of 12
`
`[Patent Claims]
`a solid polymer electrolyte memb
`{Claim 1] A joined body formed by sandwiching
`a
`rane
`a power supply for applying
`to 2 gas
`2 gas diffusion electrodes,
`by
`voltage
`diffusion electrodes of the joined body, and a
`hydrogen supply system for supplyi
`ng a
`hydrogen hydrate gas to a gas diffusion electrode side connected to a
`positiv
`: a gas
`e electrode of the power supply ; A
`hydrogen boosting device, comprising
`diffusion electrode connected to a
`negative electrode of a power supply ; andah
`a
`ydrogen discharge path for extracting
`high pressure hydrogen gas from the gas
`diffusion electrode.
`hydrogen gas are
`[Claim 2] In the fuel cell, hydrogen gas and a
`supplied respecti
`to the hydrogen electrode and the oxygen electrode on both sides of a
`vely
`joined
`a solid polymer electrolyte membrane with 2
`body which is joined by sandwiching
`A fuel cell according
`to claim 1,
`gas diffusion electrodes, and power is generated.
`to the hydrogen electrode is provided with
`wherein the hydrogen gas supply path
`the hydrogen boosting device of claim 1, and the hydrogen gas of high pressure f
`rom the hydrogen discharging path of the hydrogen boosting device is supplied
`to
`the hydrogen electrode.
`
`
`
`[Detailed description of the invention]
`
`f[0001}
`[Industrial field of application] The present invention relates to a
`ng device and a fuel cell using the same.
`
`hydrogen boosti
`
`[0002}
`{Prior art] Fuel cells have been used as
`relatively small power plants, e.g., buildin
`g units and plant units, because they have excellent characteristics such as no ne
`ed to use fossil fuels with resource
`depletion problems, little noise, and very high
`energy recovery efficiency compared to other energy engines. In recent years, it
`has been considered that this fuel cell is utilized as a power supply for a motor w
`an
`hich operates in place of an internal combustion engine mounted on a
`vehicle,
`da vehicle or the like is driven by this motor. In this case, it is important to reuse
`as is obvious from the
`the material produced by the reaction as much as
`possible,
`fact that it is mounted on a vehicle. While a much larger output is not required, it
`is desirable to be as small as
`possible with all ancillary equipment, and fuel cells e
`
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`2021/04/12
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`Patent/Utility Model Document Display | J-PlatPat [JPP]
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`Page 5 of 12
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`mploying
`
`an ion exchange membrane have attracted attention from such point of
`
`view.
`
`as an
`
`a basic structure of a solid polymer electrolyte memb
`[O003}Here,
`example,
`rane fuel cell body will be described with reference to FIG. 3. As shown in FIG. i,
`the battery body O1 is constituted by bonding gas diffusion electrodes 03 A and 0
`3 B to both sides of a solid polymer electrolyte membrane 02. This bonded body i
`s manufactured by laminating gas diffusion electrodes 03 A and 03 B on both side
`s of the solid polymer electrolyte membrane 02, and then performing hot pressin
`g or the like. Further, the gas diffusion electrodes 03 A and 03 B are formed by b
`onding the reaction films 04 A and G4 B and the gas diffusion films 05 A and 05
`B, respectively, and the surfaces of the reaction films 04 A and 04 B are in contac
`a cell reaction occurs
`t with the electrolyte film 02. Thus,
`mainly at the interface
`between the electrolyte membrane Q2 and the reaction membranes 04 A, 04 B. O
`n the surface of the gas diffusion electrode 03 A,
`an oxyg
`a gas separator having
`en
`supply groove 06 a is provided, and on the surface of the other gas diffusion el
`a
`hydrogen supply groove Q7 A is provided.
`ectrode 03 B,
`
`A gas separator 07 is joined, and constitutes an oxygen electrode and a
`electrode.
`[0004]Then, when the oxygen supply groove 06 a and the hydrogen supply groov
`are
`e 07 a
`supply oxygen and hydrogen, respectively, oxygen and hydrogen
`suppl
`ied to the reaction films 04 A and 04 B through the gas diffusion films 05 A and 0
`5 B, respectively, and the following reaction occurs at the interface between the r
`eaction films 04 A and 04 B and the electrolyte film 02.
`Interface of the reaction film O4A:
`
`hydrogen
`
`O02 +4H+ +46€->2H20
`
`Interface of the reaction film O4B:
`
`2H2—7~4H4e.
`
`Here, 4 H flows through the electrolyte membrane 02 from the hydrogen electrod
`-
`e to the oxygen electrode ; however, 4 e
`flows from the hydrogen electrode tot
`he oxygen electrode through the load 08, thereby obtaining electric energy.
`
`{0005}
`[Problem to be solved by the invention] In such a fuel cell,
`hydrogen
`to a
`ial reformed gas obtained by mainly reforming methanol is supplied
`hydroge
`n
`raw material reformed gas
`electrode, but there is a
`problem that the hydrogen
`raw material reformed gas. In
`contains CO 2 and CO in addition to the hydrogen
`other words, in order to increase the output density of the fuel cell and improve t
`he performance, it is effective to remove the impurity gas such as CO in the hydr
`ogen source reformed gas and to improve the partial pressure of the hydrogen ga
`
`raw mater
`
`a
`
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`Page 6 of 12
`
`S.
`
`{OOQ6]In view of such circumstances, it is an
`object of the present invention to pr
`ovide an
`apparatus capable of increasing hydrogen pressure and a fuel cell using
`the same.
`
`to the p
`
`{0007}
`{Means for solving the problem] The hydrogen boosting device according
`resent invention for achieving the above object is characterized in that a
`joined b
`a solid polymer electrolyte membrane between 2 gas
`ody formed by sandwiching
`a power supply for applying
`a
`to 2 gas diffusion elect
`diffusion electrodes,
`voltage
`rodes of the joined body, and a
`a
`hydrogen supply system for supplying
`hydrogen
`hydrate gas to a gas diffusion electrode side connected to a
`positive electrode of t
`are
`provided. The fuel cell according to the present invention is c
`he power supply
`haracterized in that it has a
`out a
`hydrogen discharge path for taking
`high pressu
`hydrogen gas from a gas diffusion electrode side connected to a
`negative elect
`rode of the power source, and a fuel cell according to the present invention. In th
`e fuel cell, hydrogen gas and a
`hydrogen gas are
`to the hyd
`supplied respectively
`rogen electrode and the oxygen electrode on both sides of a
`joined body which is
`a solid polymer electrolyte membrane with 2 gas diffusion
`joined by sandwiching
`A
`electrodes, and power is generated.
`hydrogen pressurizing device having the ab
`ove constitution is interposed in the hydrogen gas supply system to the hydrogen
`electrode, and the hydrogen gas of high pressure from the hydrogen discharging
`system of the hydrogen boosting device is supplied to the hydrogen electrode.
`
`re
`
`[0008}
`to 2 gas diffusion electrodes of a
`[Action and effect] When a
`voltage is applied
`joi
`ned body with a solid polymer electrolyte membrane sandwiched between 2 gas d
`iffusion electrodes and a gas diffusion electrode side connected to a
`positive elect
`on the positive
`rode is supplied with a
`hydrous gas, a next reaction is generated
`e
`lectrode side and the negative electrode side.
`:
`Positive electrode ()
`~
`H 2
`
`2H Ze.
`
`(low pressure)
`Anode (-):
`
`2H2e-—H 2
`
`a
`
`(high pressure).
`I of the positive electrod
`relationship between the pressure (PH 2)
`[0009}Then,
`e
`side, the pressure (PH 2) II of the negative electrode side, and the voltage is re
`presented by the Nernst equation of the following Equation 1.
`
`[0010]
`{Mathematical formula 1]
`
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`Patent/Utility Model Document Display | J-PlatPat [JPP]
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`Page 7 of 12
`
`Li
`
`(P no)
` E« In
`CP ads
`
`{OOL1}It is found that the hydrogen pressure (PH 2) II on the negative electrode
`side increases when the voltage is increased than the Nernst equation, and, for e
`in order to increase the pressure by 10 times, the voltage is increased by
`xample,
`10 times.
`
`{O0012]In addition, in the hydrogen boosting device of the present invention, only
`so that CO and CO 2 are
`hydrogen is taken out from the negative electrode side,
`removed as a result. However, since CO lowers the catalytic activity of the gas dif
`fusion electrode on the positive electrode side, it is necessary to remove CO by, f
`or
`example, changing the CO to CO 2 beforehand.
`
`[0013]
`{Examples} Hereinafter, the present invention will be described based on
`Ss.
`
`Example
`
`conceptually shows a
`[OO14}FIG. 1
`hydrogen boosting device according
`bodiment. As shown in FIG. 4, the hydrogen booster 100 has a structure in which
`a solid polymer electrolyte membrane 101 is sandwiched between 2 gas diffusion
`electrodes 102 A and 102 B and bonded together. Here, the gas diffusion electrod
`es 102 A and 102 B include reaction films 103 A and 103 B and gas diffusion films
`104 A and 104 B, respectively. Then, the joined body is sandwiched between the
`gas separator 105,106 and the gas separator 105,106, and a power source 107 is
`connected to the gas separator 1. Note that the gas separator 105,106 has a
`hyd
`rogen supply groove 105 a
`(in the case where the water supply groove is not for
`med at the same time when the hydrogen-containing gas is not humidified) and a
`hydrogen discharge groove 106 a.
`[QO0i5]Iin this embodiment, the gas diffusion electrodes 102 A and 102 B have rea
`an average particle diamete
`ction films 103 A and 103 B in which platinum having
`r of 50 A and a
`an average particle diameter of 4
`hydrophilic carbon black having
`a
`hydrophobic carbon black and a
`an avera
`50 A,
`polytetrafluoroethylene having
`ge particle diameter of 0.3 um are formed ata ratio of 0.7 : 7: 3: 3. A
`an average particle diameter of 420 A and a
`obic carbon black having
`polytetrafi
`an average particle diameter of 0.3 pm are
`composed of hy
`
`to an em
`
`hydroph
`
`uoroethylene having
`
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`Page 8 of 12
`
`drophobic gas diffusion films 104 a and 104 b consisting of 7:3 ratio. The reaction
`films 103 a and 103 b and the hydrophobic gas diffusion films 104 a and 104 b ar
`an
`a
`a
`e made of a solvent naphtha,
`hydrocarbon, and a mixture o
`alcohol,
`fF raw materials other than platinum.
`
`water,
`
`a solvent such as an element and then compacting t
`It can be obtained by mixing
`superposed and rolled, and a Pt 0.56mg/cm2 is supp
`he mixture. Then, these are
`orted on the side of the reaction films 103 A and 103 B by the platinum chloride r
`edox method, whereby the gas diffusion electrodes 102 A and 102 B are manufac
`a
`tured. As the solid polymer electrolyte membrane 101,
`perffuorosulfonic acid po
`117 : manufactured by DuPont Co., Ltd.) having
`a thick
`lymer membrane (Nafion
`ness of 0.17 was used. Then,
`a solid polymer electrolyte membrane 101 is sandwi
`ched between the gas diffusion electrodes 102 A and 102 B, and hot pressed
`to fo
`rm a
`2 metallic gas separators 105,1
`joined body, which is further sandwiched by
`06 and, and a power source 107 is connected to form a
`hydrogen booster 100.
`{[0016]When humidified H 2 gas was
`to the gas separator 106 using the
`supplied
`a
`high-pressure hydrogen gas of 10 atm was obtained fro
`hydrogen booster 100,
`m the hydrogen discharge groove 106 a of the gas separator 105. In this case, th
`e condition was 0.25 V in the 1.00A/cm2.
`[OO17}FIG. 2 shows an
`example of a fue! cell system incorporating the hydrogen
`booster 100. As shown in FIG. 4, the methanol reformed gas supplied
`to the hydr
`ogen electrode 12 of the fuel cell main body 11 is produced by the methanol refor
`ming apparatus 13. The methanol reformer 13 is composed of a
`reforming part 1
`4 and a
`preheating part 15, and the reforming part 14 is heated by combustion of
`a combustion gas consisting of an unreacted gas and air from a
`hydrogen electro
`an exhaust gas of a combustion gas
`de 12, and a
`preheating part 15 is heated by
`heated in the reforming part 14. The preheating unit 15 is connected to the meth
`anol tank 17 via a
`reforming methanol supply pipe 16, and a pump 20 for driving
`as a raw
`the motor 19 for feeding methanol 18 in the methanol tank 17 serving
`material of the reformed gas to the methanol reforming unit 13 is attached to the
`middle of the reforming methanol supply pipe 16. Also, in the middie of the meth
`ano! supply pipe 16 for reforming The other end side of the water supply pipe 22
`communicating with the water tank 21 is connected to one end side, and a pump
`25 for driving the motor 24 for feeding the water 23 in the water tank 21 serving
`as a
`me
`raw material together with the methanol 18 into the reforming
`reforming
`thanol supply pipe 16 is attached in the middle of the water
`supply pipe 22.
`[0018]Therefore, while passing through the preheating pipe 26 in the preheating
`raw material composed of methanol 18 and water 23 is pre
`unit 15, the reforming
`°
`°
`heated to about 200
`C. to 500
`C. by heat exchange with the high-temperature
`
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`

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`Page 9 of 12
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`combustion exhaust gas generated by combustion of the combustion gas. Then, t
`raw material is gasified in the reforming section 14 and p
`he preheated reforming
`asses
`through the reforming gas generating tube 27, and comes into contact with
`the reforming catalystfilled in the reforming gas generating tube 27 under heatin
`g, and is reformed by the next reforming reaction.
`
`CH3 OH+nH2 O
`
`>
`
`However, 0 <<1.
`
`(1 -) CO nCO 2 (2) H 2.
`
`In such a
`
`modification, the mixing ratio of methanol 18 to water 23 is 1 mol of m
`ethanol, and 0. 05. 0 of water is added to methanol.
`
`It is desirable to set the molar ratio to about 5 mole. In addition, in order to effici
`ently carry out the reforming reaction of the raw material gas, reformed gas is ref
`ormed.
`
`It is desirable to set the pressure in the production pipe 27 to about 0 kg weight t
`o about 20 kg weight per square centimeter and to set the temperature in the ref
`°
`°
`C. to about 600
`orming gas generation pipe 27 to about 200
`C. As the reformi
`one
`containing at least one element among piatinum (P
`ng catalyst, for example,
`or one
`containing at least
`t) and palladium (Pd) and rhodium (Rh) and nickel (Ni),
`one element among copper (Cu) and zinc (Zn) and chromium (Cr} may be used.
`[OQ019]Iin addition, when the methanol reformer 13 is started, the methanol 18 in
`the methanol tank 17 is supplied instead of the unreacted gas from the battery b
`a
`ody 11 used as the combustion gas. In other words,
`starting methanol supply pi
`pe 28 connecting the reforming section 14 and the methanol tank 17 is provided,
`and a
`starting device 29 is provided in the middie of the starting methanol supply
`pipe 28. The starting device 29 is a
`starting fuel supply pump (not shown) for fee
`ding the methano! 18 in the methanol tank 17 to a nozzle portion (not shown) in
`the reforming unit 14. It is provided with a methanol vaporizer (not shown) for va
`porizing the methanol 18 supplied from the starting fuel supply pump and feeding
`it Into a nozzle portion (not shown).
`a 1 CO reduction device 30 is provided
`[0020}0n the other hand,
`nicate with the reformed gas outlet side of the methanol reformer 13. The 1 COr
`educing device 30 is filled with a CO shift catalyst for reducing CO in the reformed
`gas generated by the reforming reaction in the reforming gas generating tube 27.
`one
`containing at least one element selecte
`As the CO shift catalyst, for example,
`d from copper (Cu) and zinc (Zn) may be used. Here, in the CO shift process in th
`e 1 CO reduction device 30, CO is converted into CO 2
`by reaction with H 2 and C
`
`so as to commu
`
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`Page 10 of 12
`
`O concentration is reduced to about 1%.
`{0021]Further, the reformed gas supply pipe 31 communicating with the 1 CO re
`duction device 30 is connected to the 2 CO reduction device 32. In this 2 CO redu
`ction device 32, by introducing air into the reformed gas, a process (SelectOxo) is
`performed in which CO which is about 1% as described above is reduced to about
`100 ppm.
`
`a reformed gas which is reduced in CO is introduced i
`[OO22]Iin this embodiment,
`nto the hydrogen booster 100, and the hydrogen gas boosted by the hydrogen bo
`oster 100 is humidified by the humidifier 33 and then introduced into the hydroge
`n electrode 12 of the fuel cell 11. In other words,
`a
`hydrogen booster 100 and ah
`umidifier 32 are mounted between the 2 CO reduction device 32 of the reformed
`
`gas supply pipe 31 and the fuel cell main body 11. Then, among the reformed ga
`excess unrea
`Ss sent into the hydrogen electrode 12 of the fuel cell main body 11,
`an unreacted gas supply pipe 34 which connects the
`cted gas is supplied through
`fuel cell main body 11 and the reforming section 14 of the methanol reforming ap
`paratus 13.
`
`to the reforming section 14.
`It is supplied
`a blower 37 is connected to an oxygen electrode 35 of
`{0623]On the other hand,
`the fuel cell main body 11 via an air supply pipe 36, and pressurized air from the
`to the
`blower 37 is fed to the oxygen electrode 35 side. Then, this air is supplied
`water / water separator 38 which is connected to the oxygen electrode 35 in a sta
`water on the side of the oxy
`te in which water is contained in the reaction product
`gen electrode 35 in the fuel cell main body 11, and the water content therein is re
`covered in the water tank 21 via the water recovery pipe 39 and is discharged fro
`m the exhaust pipe 40.
`a blower drive motor 42 supplied with ele
`[0024]Here, the blower 37 is driven by
`ctricity from a
`as a power source. In addition, electricit
`41 serving
`storage battery
`an exhaust turbine 43 interpo
`y generated by the generator 44 which is driven by
`sed in the reformed gas supply pipe 31 between the 1 CO reduction device 30 an
`a 2 ai
`41. Further,
`d the 2 CO reduction device 32 is stored in the storage battery
`r
`supply pipe 45 branching from the air supply pipe 36 from the blower 37 is com
`municated with the middle of the methanol supply pipe 28, and air which become
`s a combustion gas in the reforming section 14 of the methano! reformer 13 is su
`pplied via the 2 air supply pipe 45 as described above. In addition, the motor 19,
`41
`to the
`24 is operated by electricity supplied from the storage battery
`blower drive motor.
`
`similarly
`
`[0025]The water tank 21, the fuel cell main body 11, and the humidifying device
`33 are connected to each other via a
`circulating pipe 46 and a coolli
`water
`
`cooling
`
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`Page 11 of 12
`
`ng water
`circulating pipe 46 between the water tank 21 and the fuel cell main bo
`a motor 47 is provided for supplying water 23 ina
`dy i1. A pump 48 for driving
`water tank 21 to a fuel cell main body 11, cooling the fuel cell main body 11, and
`water to a
`humidifying device 33. In addition, in the h
`sending the heated cooling
`umidifying device 33, the reformed gas flowing in the reformed gas supply pipe 3
`water come into contact with each other via a gas diffusi
`1 and the heated cooling
`on
`film, and steam is added to the reformed gas at a steam partial pressure corre
`water. Further, the motor 47i
`to the temperature of the heated cooling
`sponding
`S
`operated by electricity of a
`storage battery.
`[0026]When generating electricity in such a fuel cell, CO in the hydrogen
`eformed gas is removed by the hydrogen booster 100 and the high pressure hydr
`ogen gas is supplied to the hydrogen electrode 12 of the fuel cell body 11, so that
`a state in which the output density is improved is maintained.
`
`source r
`
`[0027]
`[Effect of the Invention] As described above, according to the hydrogen boosting
`an
`device of the present invention, high pressure hydrogen gas is easily obtained,
`d when the high pressure hydrogen gas is applied to a fuel cell, the reduction ina
`on the
`ctivity due to the CO poisoning caused by the CO poisoning of the catalyst
`hydrogen electrode side is prevented, and good power generation with improved
`current density is achieved.
`
`
`
`[Brief Description of the Drawings]
`[Fig. 1]FIG. 1 is a schematic diagram of a
`an embodiment ;.
`
`hydrogen boosting device according
`
`to
`
`a fuel cell system according
`
`to a
`
`example of a fuel cell body.
`
`[Fig. 2]FIG. 1 is a schematic diagram illustrating
`nm embodiment ;.
`[Fig. 3]It is an
`explanatory view showing
`[Expianation of letters or
`numerals]
`1 reformed gas supply pipe
`tower
`2 a, 2 b adsorbent packed
`6 a, 6 b air inlet pipe
`8A, 8B
`Exhaust pipe
`
`an
`
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`

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`Patent/Utility Model Document Display | J-PlatPat [JPP]
`
`Page 12 of 12
`
`11
`
`Fuel Cell Body
`12 Hydrogen Pole
`13 methanol reformer
`
`i4
`
`Reforming Section
`15 Preheating Part
`16 reforming methanol! supply pipe
`17 Methanol Tank
`
`18 Methanol
`
`21 Water Tank
`
`23 Water
`
`30 1 CO reduction device
`
`31 reformed gas supply pipe
`32 2 CO reduction device
`
`33 humidifier
`
`35 Oxygen Pole
`36 Air Feed Pipe
`100 hydrogen boosting device
`101 solid polymer electrolyte membrane
`102A,102B gas diffusion electrode
`103A,103B reaction film
`
`104A,104B
`105,106 Gas separator
`107 Power Supply
`
`
`
`Copyright JPO and INPIT
`
`(P0201)
`
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`
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`
`

`

`Cs) pee CIPD
`
`a2)
`
`gS BR oe at ty BRA)
`
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