WO2010125732A1 - 燃料電池用改質装置 - Google Patents
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- WO2010125732A1 WO2010125732A1 PCT/JP2010/001570 JP2010001570W WO2010125732A1 WO 2010125732 A1 WO2010125732 A1 WO 2010125732A1 JP 2010001570 W JP2010001570 W JP 2010001570W WO 2010125732 A1 WO2010125732 A1 WO 2010125732A1
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Definitions
- the present invention relates to a reformer for a fuel cell that reforms raw fuel to generate a reformed gas used in a fuel cell.
- a polymer electrolyte fuel cell has a basic structure in which a polymer electrolyte membrane, which is an electrolyte membrane, is disposed between a fuel electrode and an air electrode.
- the fuel electrode contains hydrogen and the air electrode contains oxygen. It is a device that supplies the agent gas and generates power by the following electrochemical reaction.
- the fuel electrode H 2 ⁇ 2H + + 2e - ⁇ (1)
- Cathode 1 / 2O 2 + 2H + + 2e - ⁇ H 2 O ⁇ (2)
- hydrogen used as a fuel for a polymer electrolyte fuel cell is a natural gas, a hydrocarbon gas such as naphtha, or a raw fuel gas of alcohols such as methanol and water vapor, which are relatively easily and inexpensively available.
- the technique obtained by mixing and reforming in the reforming section is employed. Hydrogen gas obtained by reforming is supplied to the fuel electrode of the fuel cell and used for power generation.
- FIG. 1 is a schematic diagram showing the configuration of a conventional fuel cell system.
- the fuel cell system 300 includes a fuel cell reformer 302 that generates hydrogen-rich reformed gas from raw fuel, and a fuel cell 400.
- raw fuel hydrogen gas such as natural gas or LPG
- LPG low-density polyethylene
- the raw fuel from which the sulfur component has been removed is supplied to the reforming unit 320.
- the reforming unit 320 steam-reforms the raw fuel by passing the raw fuel through the catalyst heated by the burner 322 to generate a reformed gas.
- the reformed gas generated by the reforming unit 320 is heat-exchanged with reformed water (steam) before being added to the raw fuel in the heat exchanging unit 340, and then supplied to the CO converting unit 350.
- carbon monoxide is converted to hydrogen by a shift reaction. Thereby, the hydrogen concentration is increased and the CO concentration is reduced.
- the reformed gas whose CO concentration has been reduced by the CO shifter 350 is heat-exchanged with the water vapor evaporated in the vaporizer 330 in the heat exchanger 342 and then supplied to the CO remover 360.
- the CO concentration is further reduced by the CO oxidation reaction using the CO selective oxidation catalyst. Note that air necessary for the CO oxidation reaction is supplied to the reformed gas whose CO concentration has been reduced by the CO conversion unit 350.
- the reformed gas whose CO concentration is further reduced by the CO removing unit 360 is supplied to the fuel electrode of the fuel cell 400 after exchanging heat with water vapor in the heat exchanging unit 344.
- Air is supplied as an oxidant to the air electrode of the fuel cell 400, and power is generated by an electrochemical reaction between hydrogen and oxygen.
- the steam necessary for the reforming reaction in the reforming unit 320 is generated from the reformed water supplied from the outside of the fuel cell system 300.
- the liquid reforming water supplied from the outside is vaporized by exchanging heat with the exhaust gas from the burner 322 in the vaporizing section 330 to become water vapor.
- the water vapor generated by the vaporization unit 330 is heat-exchanged with the reformed gas in the order of the heat exchange unit 342, the CO removal unit 360, and the heat exchange unit 344, and then the reformed gas in the order of the CO conversion unit 350 and the heat exchange unit 340. After further heat exchange, it is mixed with the desulfurized raw fuel.
- the inlet side of the reformer for the fuel cell ( The raw fuel supply port) and the outlet of the reformer for the fuel cell (the outlet part of the reformed gas) are closed, the raw fuel is introduced from the inlet of the reformer for the fuel cell, and the reformer for the fuel cell
- a method for purging the gas flow path of the apparatus a method for purging the gas flow path of the fuel cell reformer by introducing air from the outlet side of the fuel cell reformer.
- the inside of the reformer for the fuel cell is depressurized due to water condensation due to a temperature drop.
- the electromagnetic valve etc. which seal the gas flow path in the reformer for fuel cells are easily damaged.
- the reaction of the reformer or the like may be heated to a temperature higher than the thermal decomposition temperature at startup. This causes a problem that coking occurs on the reforming catalyst and the catalyst performance is lowered.
- the selective oxidation catalyst of the CO removal unit may be oxidized by the inflow of air.
- the selective oxidation catalyst of the CO removal unit may be oxidized by the inflow of air.
- a sacrificial oxidant is provided on the downstream side of the selective oxidation catalyst, air remains in the gas flow path from the downstream side of the sacrificial oxidant to the outlet side of the fuel cell reformer to which air is introduced. To do. For this reason, when the reforming device for a fuel cell is started, the air remaining in the gas flow channel flows into the fuel cell, whereby the oxidation of the catalyst metal used for the electrode of the fuel cell proceeds, and the fuel cell The durability of is reduced.
- the present invention has been made in view of these problems, and the object thereof is to reduce the degradation of the selective oxidation catalyst with a simple configuration when the fuel cell reformer is stopped without causing a decrease in the durability of the fuel cell. It is to provide technology that can be suppressed.
- An embodiment of the present invention is a fuel cell reformer.
- the fuel cell reformer reduces the CO concentration of the reformed gas generated in the reforming unit and reforming unit that reforms the raw fuel to generate reformed gas mainly composed of hydrogen by shift reaction.
- An air supply unit capable of introducing air into the gas flow channel via the air supply flow channel, and after stopping the supply of raw fuel to the reforming unit, the gas upstream of the CO removal unit Air is introduced into the flow path.
- the reforming section and the CO conversion section are higher in temperature and larger in volume than the CO removal section. For this reason, when the fuel cell reforming apparatus is shut down, the reforming section and the CO conversion section are more affected by water condensation and temperature drop, and the interior of the reforming section and the CO conversion section is compared to the CO removal section. It becomes easy to be decompressed. As a result, the air introduced into the gas flow path on the upstream side of the CO removal unit can easily flow into the CO conversion unit side. Oxygen in the air is removed from the air that has flowed into the CO conversion section by oxidation of the shift catalyst. The air from which oxygen has been removed naturally flows into the reforming section.
- the volume of the gas flow path from the CO conversion section to the location where the air supply flow path is connected is from the location where the air supply flow path is connected to the CO removal section. It may be smaller than the volume of the gas flow path.
- the volume of the gas flow path from the CO transformation section to the location where the air supply flow path is connected is 1/6 or less of the volume of the gas flow path from the location where the air supply flow path is connected to the CO removal section It may be.
- the part of the air supply channel connected to the gas channel may also serve as a path for supplying air used for selective oxidation in the CO removal unit.
- a diffusion part for diffusing the gas flow may be provided in the gas flow channel located on the downstream side with respect to the location where the air supply flow channel is connected.
- the air supply unit may have a normally open type on-off valve.
- the deterioration of the selective oxidation catalyst can be suppressed with a simple configuration when the fuel cell reforming apparatus is stopped, without causing deterioration of the durability of the fuel cell.
- FIG. 2 is a schematic diagram showing the configuration of the fuel cell system 100 including the fuel cell reforming apparatus 10 according to the embodiment.
- the fuel cell reforming apparatus 10 includes a desulfurization unit 20, a reforming unit 30, a burner 32, a vaporization unit 40, a heat exchange unit 50, a CO conversion unit 60, and a CO removal unit 70.
- raw fuel hydrocarbon gas such as natural gas or LPG
- the sulfur component acts as a catalyst poison for the catalyst contained in the reforming unit 30 and the fuel cell 12, and the reforming performance of the fuel cell reforming device 10 and the power generation performance of the fuel cell 12 are affected by sulfur poisoning. Decrease is suppressed.
- the desulfurization unit 20 performs desulfurization of the raw fuel by a so-called hydrodesulfurization method that removes the sulfur component by reacting the raw fuel containing the sulfur component with hydrogen in the presence of the catalyst.
- the supply amount of the raw fuel is appropriately controlled by adjusting the output of the raw fuel supply pump 14.
- An on-off valve 16 is provided on the downstream side of the raw fuel supply pump 14, and the inflow of the raw fuel can be blocked by closing the on-off valve 16.
- Raw fuel from which sulfur components have been removed is supplied to the reforming unit 30.
- the reforming unit 30 has a catalyst layer made of a reforming catalyst in which a metal catalyst such as ruthenium (Ru) is supported on a carrier such as alumina.
- a metal catalyst such as ruthenium (Ru)
- the raw fuel is steam reformed under the reforming catalyst heated by the burner 32, and a reformed gas containing about 80% of hydrogen (fuel) is generated.
- the reaction temperature during steam reforming is, for example, in the range of about 650 ° C. to 700 ° C.
- a part of the raw fuel is supplied to the burner 32 in order to raise the temperature of the reforming unit 30.
- the fuel cell 12 can be stably operated, the supply of the raw fuel to the burner 32 is stopped, and the battery off gas discharged from the fuel cell 12 is supplied to the burner 32, whereby the temperature of the reforming unit 30 is increased. Is planned.
- the exhaust gas generated by the combustion of the burner 32 is discharged from the fuel cell system 100 to the outside after exchanging heat with the reforming water in the vaporization section 40. Further, air is supplied to the burner 32 and used for combustion of the burner 32.
- the reformed gas generated by the reforming unit 30 is supplied to the CO conversion unit 60 after exchanging heat with water vapor that has passed through the vaporization unit 40 when passing through the heat exchange unit 50.
- the CO conversion unit 60 has a catalyst layer made of a Cu—Zn-based catalyst made of, for example, copper oxide or zinc oxide pellets.
- carbon monoxide is converted to hydrogen by a shift reaction. Thereby, the hydrogen concentration of the reformed gas is increased and the CO concentration is reduced to 0.5% or less.
- the CO selective oxidation reaction is performed, for example, in the range of about 70 ° C. to 180 ° C.
- FIG. 3 shows a specific example of the diffusion unit 80.
- the diffusion unit 80 is a twist plate that is formed by twisting a flat plate-like member and is installed in a gas flow path (pipe) from the CO conversion unit 60 to the CO removal unit 70.
- the gas passes through the pipe in which the diffusing unit 80 is provided, the gas collides with the diffusing unit 80, whereby the gas diffusibility is enhanced.
- the reformed gas and the selective oxidation air pass through the pipe provided with the diffusion portion 80, so that the reforming gas and the selective oxidation air can be mixed (mixed) and gas dispersible. Can be improved.
- the entire selective oxidation catalyst used in the CO removing unit 70 can be efficiently contributed to CO removal, and thus the durability of the CO removing unit 70 can be improved.
- the CO removal unit 70 can be made compact while the lifetime of the CO removal unit 70 is equal.
- the CO removing unit 70 has a catalyst layer made of a CO selective oxidation catalyst in which Ru is supported on a carrier such as alumina, and the reformed gas is formed by a CO oxidation reaction using the CO selective oxidation catalyst.
- the CO concentration is reduced to about 10 ppm.
- air necessary for the CO oxidation reaction is supplied to the reformed gas whose CO concentration has been reduced by the CO conversion unit 60.
- the air supply flow path 102 is connected to a gas flow path located upstream of the diffusion section 80.
- the air supply flow path 102 is branched into two parts, an air supply flow path 102a and an air supply flow path 102b.
- air is supplied to the gas flow channel located upstream of the diffusion unit 80 via the air supply flow channel 102 a, and the CO oxidation reaction in the CO removal unit 70 is performed. Used.
- the air supply channel 102 a is provided with an air supply pump 104 and an on-off valve 106, and the supply amount of air can be adjusted by controlling the output of the air supply pump 104. Further, by closing the on-off valve 106, the inflow of air to the gas flow channel located upstream of the diffusing unit 80 is blocked.
- an on-off valve 108 is provided in the air supply channel 102a.
- the on-off valve 108 is specifically a normally open type electromagnetic valve. That is, the on-off valve 108 is closed during the operation of the fuel cell reforming apparatus 10, but when the operation of the fuel cell reforming apparatus 10 is stopped, the on-off valve 108 is opened to supply air. Air is supplied to the gas flow channel located on the upstream side of the diffusing section 80 via the use flow channel 102b.
- the volume of the gas flow path from the CO transformation section 60 to the location where the air supply flow path 102 is connected is the volume of the gas flow path from the location where the air supply flow path 102 is connected to the CO removal section 70. It is desirable that it is small compared. More desirably, the volume of the gas flow path from the CO transformation section 60 to the location where the air supply flow path 102 is connected is such that the gas flow from the location where the air supply flow path 102 is connected to the CO removal section 70. 1/6 or less of the volume of the road.
- the gas flow path from the location where the air supply flow path 102 is connected to the CO removal section 70 is more effective from the CO transformation section 60 to the air.
- the supply channel 102 is longer than the gas channel up to the connected location. According to this configuration, the reformed gas, the reformed gas, and the air for selective oxidation pass through the gas flow path from the location where the air supply flow path 102 is connected to the CO removal unit 70 to mix them. Can be improved.
- the volume of the gas flow path from the CO transformation section 60 to the location where the air supply flow path 102 is connected is preferably 10 cm 3 or less.
- a typical example of the volume of the gas flow path from the CO transformation section 60 to the location where the air supply flow path 102 is connected is 6 cm 3 .
- a typical example of the volume of the gas flow path from the location where the air supply flow path 102 is connected to the CO removing unit 70 is 43.5 cm 3 .
- the diameter of the gas flow path provided between the CO conversion unit 60 and the CO removal unit 70 is preferably 6 to 12 mm, typically 3/8 inch.
- the reformed gas whose CO concentration is further reduced by the CO removing unit 70 is supplied to the fuel electrode of the fuel cell 12.
- An on-off valve 18 is provided on the downstream side of the CO removing unit 70, and the gas flow from the CO removing unit 70 to the fuel cell 12 can be blocked by closing the on-off valve 18.
- the fuel cell 12 is, for example, a solid polymer fuel cell, and is a laminate in which a plurality of membrane electrode assemblies (single cells) each having a solid polymer electrolyte membrane provided between a fuel electrode and an air electrode are laminated. Have. Air is supplied to the air electrode of the fuel cell 12 as an oxidant, and power is generated by an electrochemical reaction between hydrogen and oxygen.
- the amount of air supplied to the air electrode of the fuel cell 12 is adjusted by controlling the output of the air supply pump 112.
- An on-off valve 110 is provided on the upstream side of the air supply pump 112, and the inflow of air to the air electrode of the fuel cell 12 can be blocked by closing the on-off valve 110.
- the water vapor necessary for the reforming reaction in the reforming unit 30 is generated from the reformed water supplied from the outside of the fuel cell system 100.
- the reformed water is generated by treating the clean water with a water treatment device (not shown) provided with a reverse osmosis membrane and an ion exchange resin.
- the water treatment device reduces the conductivity of clean water and suppresses the mixing of organic substances.
- the supply amount of the reforming water is appropriately controlled by adjusting the output of the reforming water supply pump 90.
- the liquid reforming water supplied from the outside is heated by exchanging heat with the reformed gas at the CO shift section 60 and then supplied to the vaporizing section 40.
- the reformed water starts to evaporate when heat is exchanged with the reformed gas in the CO shift section 60. Further, vaporization is completed by exchanging heat with the exhaust gas from the burner 32 in the vaporization section 40.
- the water vapor vaporized in the vaporization unit 40 is heated to become superheated steam when passing through the heat exchange unit 50 and then added to the raw fuel on the downstream side of the desulfurization unit 20.
- the raw fuel supply pump 14 is driven, the on-off valve 16 is opened, and the raw fuel is supplied to the desulfurization unit 20.
- the raw fuel is desulfurized in the desulfurization unit 20 and then supplied to the reforming unit 30 together with steam, and a reformed gas containing hydrogen is generated by the reforming reaction.
- the reformed gas generated in the reforming unit 30 passes through the heat exchanging unit 50 and is then supplied to the CO conversion unit 60, so that the CO concentration in the reformed gas is reduced by a shift reaction.
- the outlet gas of the shift reaction unit is supplied to the CO removal unit 70.
- the on-off valve 106 is opened and the air supply pump 104 is driven, whereby the air for selective oxidation reaction is supplied to the gas flow path on the upstream side of the diffusion unit 80.
- the on-off valve 108 is closed.
- the on-off valve 18 is opened, and the reformed gas containing hydrogen is supplied to the fuel cell 12.
- the on-off valve 110 is opened and the air supply pump 112 is driven to supply air to the fuel cell 12.
- the supply of air for the selective oxidation reaction is stopped by closing the on-off valve 106, and the supply of air to the fuel cell 12 is stopped by closing the on-off valve 110. Further, the supply of the reformed gas to the fuel cell 12 is stopped by closing the on-off valve 18. Further, when the power supply to the on-off valve 108 is stopped, the on-off valve 108 is opened, so that the air supply channels 102 and 102b are opened to the atmosphere. As a result, as the temperature of the fuel cell reforming apparatus 10 decreases, air flows from the air supply channel 102 into the gas channel between the CO conversion unit 60 and the CO removal unit 70.
- the volume of the gas flow path from the CO transformation section 60 to the location where the air supply flow path 102 is connected is the gas from the location where the air supply flow path 102 is connected to the CO removal section 70.
- the volume smaller than the volume of the flow path the air that has flowed into the gas flow path from the air supply flow path 102 can easily flow toward the CO shift section 60, and the shift catalyst is oxidized in the CO shift section 60. Oxygen in the air is removed.
- the air from which oxygen has been removed naturally flows into the reforming unit 30.
- the inside of the fuel cell reforming device 10 is prevented from becoming negative pressure without purging the gas flow path in the fuel cell reforming device 10, and sacrificial oxidation is performed downstream of the CO removal unit 70.
- the oxidation of the selective oxidation catalyst used for the CO removing unit 70 can be suppressed without installing an agent.
- the present invention can be used in a fuel cell reforming apparatus that reforms raw fuel to generate reformed gas mainly composed of hydrogen gas.
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Health & Medical Sciences (AREA)
- Fuel Cell (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
Description
空気極:1/2O2+2H++2e-→H2O・・・・(2)
実用的には、固体高分子形燃料電池の燃料となる水素は、比較的容易かつ安価に入手可能な天然ガス、ナフサ等の炭化水素系ガスまたはメタノール等のアルコール類の原燃料ガスと水蒸気とを混合して、改質部で改質することで得る手法が採用されている。改質により得られた水素ガスは燃料電池の燃料極に供給され、発電に用いられる。
燃料電池用改質装置10の起動時には、原燃料供給ポンプ14が駆動されるとともに、開閉弁16が開放され、脱硫部20に原燃料が供給される。原燃料は脱硫部20で脱硫された後、水蒸気とともに改質部30に供給され、改質反応により水素を含む改質ガスが生成される。改質部30で生成した改質ガスは熱交換部50を通過した後、CO変成部60に供給され、改質ガス中のCO濃度がシフト反応により低減される。シフト反応部の出口ガスはCO除去部70に供給される。また、開閉弁106が開放されるとともに、空気供給用ポンプ104を駆動させることにより、選択酸化反応用の空気が拡散部80の上流側のガス流路に供給される。なお、このとき、開閉弁108は閉じられている。また、開閉弁18は開放されており、水素を含む改質ガスが燃料電池12に供給される。燃料電池12への改質ガスの供給が開始された後、開閉弁110が開放されるとともに、空気供給用ポンプ112を駆動させることにより、燃料電池12に空気が供給される。
次に、燃料電池用改質装置10を停止する場合の手順について説明する。燃料電池用改質装置10の停止に際して、まず、原燃料供給ポンプ14の駆動が停止されるとともに、開閉弁16を閉じることにより、燃料電池用改質装置10への原燃料の供給が停止される。これと並行して、改質水供給ポンプ90の駆動が停止され、燃料電池用改質装置10への改質水の供給が停止される。また、バーナー32の燃料用の燃料および空気の供給が停止される。
Claims (6)
- 原燃料を改質して水素を主成分とする改質ガスを生成する改質部と、
前記改質部で生成した改質ガスのCO濃度をシフト反応により低減するCO変成部と、
前記CO変成部によりCO濃度が低減された改質ガスのCO濃度を選択酸化触媒を用いてさらに低減するCO除去部と、
前記CO除去部の上流側のガス流路に接続された空気供給用流路を経由して、前記ガス流路に空気を導入可能な空気供給部と、
を備え、
前記改質部への原燃料の供給を停止した後、前記CO除去部の上流側のガス流路に空気が導入されることを特徴とする燃料電池用改質装置。 - 前記CO変成部から、前記空気供給用流路が接続された箇所までのガス流路の容積が、前記空気供給用流路が接続された箇所から前記CO除去部までのガス流路の容積に比べて小さい請求項1に記載の燃料電池用改質装置。
- 前記CO変成部から、前記空気供給用流路が接続された箇所までのガス流路の容積が、前記空気供給用流路が接続された箇所から前記CO除去部までのガス流路の容積の1/6以下である請求項2に記載の燃料電池用改質装置。
- 前記ガス流路に接続された部分の前記空気供給用流路は、前記CO除去部における選択酸化に用いられる空気を供給するための経路を兼ねている請求項1乃至3のいずれか1項に記載の燃料電池用改質装置。
- 前記空気供給用流路が接続された箇所に対して下流側に位置する前記ガス流路にガスの流れを拡散する拡散部が設けられている請求項4に記載の燃料電池用改質装置。
- 前記空気供給部は、ノーマルオープン型の開閉弁を有する請求項1乃至5のいずれか1項に記載の燃料電池用改質装置。
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EP10769434.1A EP2426770A4 (en) | 2009-04-28 | 2010-03-05 | REFORMER FOR FUEL CELL |
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JP2009110059A JP5466871B2 (ja) | 2009-04-28 | 2009-04-28 | 燃料電池用改質装置 |
JP2009-110059 | 2009-04-28 |
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JP (1) | JP5466871B2 (ja) |
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Cited By (1)
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US20150152113A1 (en) * | 2012-06-21 | 2015-06-04 | Bristol-Myers Squibb Company | Positive Allosteric Modulators of MGLUR2 |
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EP2426770A1 (en) | 2012-03-07 |
JP2010257916A (ja) | 2010-11-11 |
KR20120029401A (ko) | 2012-03-26 |
EP2426770A4 (en) | 2013-05-29 |
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