JPH1072202A - Method for removing carbon monoxide in reformed gas and device therefor - Google Patents

Abstract

PROBLEM TO BE SOLVED: To efficiently and selectively remove carbon monoxide contained in a reformed gas and to prevent the poisoning of an electrode of a fuel cell due to carbon monoxide. SOLUTION: Reactors 10a, 10b, 10c...10n provided with catalyst layers 12a, 12b, 12c...12n of a carbon monoxide selective oxidation catalyst ate provided in multistage in a reformed gas conduit 14, in which the reformed gas containing carbon monoxide flows, a reformed gas temp. control means 16 for controlling a temp. to that suitable for the reaction by cooling the reformed gas in an outlet of each catalyst layer is provided in the reformed gas conduit 14 and an oxidizing gas distributing and supplying means 18 is provided between the reformed gas temp. controlling means 16 and each catalyst layer in the reformed gas conduit 14. As the catalyst, a ruthenium catalyst is preferably used.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for selectively and efficiently removing carbon monoxide (hereinafter, appropriately referred to as CO) contained in a reformed gas and an apparatus for performing the method.

[0002]

2. Description of the Related Art Conventionally, a methanol reforming reaction (CH
A method is known in which hydrogen is produced from ₃ OH + H ₂ O → CO ₂ + 3H ₂ ) and used as fuel for a fuel cell. However, for the fuel cell electrodes poisoned by CO and deteriorating the performance, such as polymer electrolyte fuel cells (PEFC) and phosphoric acid fuel cells (PAFC), the reforming reaction reverse shift reaction of CO ₂ by-reactions (CO ₂ + H
₂ → CO + H ₂ O) must be selectively removed. Known methods include selectoxo,
There are methods such as methanation, membrane separation, adsorption separation, and electrode oxidation.

[0003] Japanese Patent Application Laid-Open No. 3-276577 discloses that CO in reformed gas is oxidized by a catalytic combustor comprising a combustion catalyst of a noble metal such as platinum which preferentially combusts CO contained in reformed gas. Burned with agent (air or oxygen)
There is described a fuel cell power generator in which a reformed gas containing almost no CO is supplied to the fuel cell.

Japanese Patent Application Laid-Open No. Hei 5-201702 discloses that a catalyst layer in which rhodium (Rh) or ruthenium (Ru) is supported on an alumina-based carrier has a temperature of about 120 ° C. or less.
A gas stream containing hydrogen and carbon monoxide and a gas stream containing oxygen are preferably mixed and flown at a temperature of about 100 ° C. or less so that the O ₂ : CO volume ratio is preferably less than 1: 1. A method and apparatus for selectively removing carbon monoxide, wherein carbon monoxide is reacted with oxygen to substantially reduce the concentration of carbon monoxide in a gas stream without substantially reacting with the above.

[0005]

Among the above-mentioned selective CO removal methods, the select oxo method uses CO + 1 / 2O _2.
→ Since the reaction of CO ₂ is an exothermic reaction, for example, when the catalyst is filled to the catalyst layer length L ₀ as shown in FIG.
As indicated by the broken line in FIG. 5, the catalyst layer temperature exceeded the upper limit temperature of the reaction, 210 ° C. (when a ruthenium-based catalyst, specifically, Ru / Al ₂ O ₃ was used as the catalyst), and CO was efficiently removed. Can not do it.

[0006] The present invention has been made in view of the above points,
The purpose is to divide the catalyst layer for select oxo reaction into two or more stages, and adjust the outlet gas temperature of each stage by cooling.
By providing means for maintaining the optimum temperature condition, and distributing and supplying an oxidizing agent (such as air or oxygen) to these decomposed catalyst layers, and maintaining the temperature distribution range per stage under the optimum condition, An object of the present invention is to provide a method and an apparatus for removing CO in a reformed gas, which improve the attainment rate and the selectivity (CO removal rate).

[0007]

In order to achieve the above object, a method for removing CO in a reformed gas according to the present invention comprises the steps of: converting a reformed gas containing carbon monoxide into two or more stages in a gas flow direction; Is a method of sequentially supplying the reformed gas at the outlet of each catalyst layer to a temperature suitable for the reaction, and adding an oxidizing agent (air or oxygen) to each catalyst layer. ) (See FIG. 1). In this method, a ruthenium-based catalyst is used as a carbon monoxide selective oxidation catalyst, and the temperature of each catalyst layer is set to 60 to
It is preferable to maintain the temperature in the range of 210 ° C, preferably 130 to 180 ° C. If the catalyst layer temperature is lower than the above range, CO in the reformed gas cannot be efficiently removed. In addition, when the above range is exceeded, the reaction amount of hydrogen gas in the reformed gas increases, and the amount of hydrogen gas of the fuel that can be supplied to the fuel cell decreases. As a ruthenium-based catalyst, Ru / A
l ₂ O ₃ , Ru / SiO ₂ , Ru / SiO ₂ —Ti
O ₂ , Ru / ZrO ₂ , Ru / zeolite, Ru / cordierite and the like can be mentioned. Further, a rhodium-based catalyst is used as a carbon monoxide selective oxidation catalyst, and the temperature of each catalyst layer is set to 130 to 210 ° C, preferably to 120 to 150 ° C.
It is preferable to maintain the temperature in the range of ° C. If the catalyst temperature is lower than the above range, CO in the reformed gas cannot be efficiently removed. In addition, when the above range is exceeded, the reaction amount of hydrogen gas in the reformed gas increases, and the amount of hydrogen gas of the fuel that can be supplied to the fuel cell decreases. Rh / Al ₂ O ₃ , Rh / SiO ₂ , Rh / SiO _{2
2 -TiO 2, Rh / ZrO 2} , Rh / zeolite, R
h / cordierite and the like.

Further, the catalyst layer in each stage is divided into a ruthenium-based catalyst layer and a rhodium-based catalyst layer, and the reformed gas is treated with the ruthenium-based catalyst layer. In some cases, treatment is performed using a catalyst layer (see FIG. 12). In this case, the temperature of the reformed gas introduced into the ruthenium-based catalyst layer is in the range of 60 to 100 ° C., and the temperature of the reformed gas introduced into the adjacent rhodium-based catalyst layer is 120 to 150 ° C.
It is preferable to be in the range of ° C. Ru / Al ₂ O ₃ , Ru / SiO ₂ , Ru / Si
O ₂ —TiO ₂ , Ru / ZrO ₂ , Ru / zeolite,
Ru / cordierite and the like. Also,
Rhodium-based catalysts include Rh / Al ₂ O ₃ and Rh / S
iO ₂ , Rh / SiO ₂ —TiO ₂ , Rh / ZrO ₂ ,
Rh / zeolite, Rh / cordierite and the like can be mentioned. The temperature of the ruthenium-based catalyst layer is 60 to 100
° C, the temperature of the rhodium-based catalyst layer is from 120 to 1
If the temperature is out of the range of 50 ° C., the C
O cannot be efficiently removed.

In these methods, the O ₂ / CO molar ratio at the inlet of each catalyst layer is 0.5 to 1.5 (oxygen stoichiometric ratio 1.0 to 3.0), preferably 0.8 to 1.0. The oxidizing agent is preferably distributed and supplied so as to be in the range of (oxygen stoichiometric ratio 1.6 to 2.0). If the O ₂ / CO molar ratio is less than the above range, there is a disadvantage that the amount of O ₂ that reacts with CO is insufficient and unreacted CO remains, while the O ₂ / CO molar ratio is lower than the above range. If the value exceeds the range, C
O react with O ₂ volume other than O ₂ was increases, since the gas temperature is raised by heat generation, there is a disadvantage that H ₂ and O ₂ in the reformed gas decreases the reaction to H ₂ gas. The catalyst layer may be a normal particle-filled layer (see FIG. 4) or a honeycomb-filled layer. However, catalyst particles are used as a catalyst, and at least one of glass beads, ceramic particles, and metal particles is mixed with the catalyst particles. (See FIG. 5).

In the apparatus for removing CO in reformed gas according to the present invention, a reactor equipped with a catalyst layer of a carbon monoxide selective oxidation catalyst is provided in multiple stages in a reformed gas conduit through which a reformed gas containing carbon monoxide flows. A reformed gas temperature adjusting means for cooling the reformed gas at the outlet of each catalyst layer and adjusting the temperature to a temperature suitable for the reaction is provided in the reformed gas conduit, and these reformed gas temperature adjusting means and each catalyst layer are An oxidizing agent distribution and supply means is provided in the reformed gas conduit between the two (see FIG. 1). In the above apparatus, the catalyst layer of each stage may be divided into two parts, a ruthenium-based catalyst layer on the upstream side and a rhodium-based catalyst layer on the downstream side (see FIG. 12).

In these apparatuses, a tubular reactor having a cylindrical body filled with a catalyst (see FIGS. 6 and 7) or a plate reactor having a catalyst filled between two plates is used as a reactor. (See FIGS. 10 and 11), or one in which a plurality of small tubes filled with a catalyst are inserted into a cylindrical main body (see FIGS. 8 and 9).

[0012]

FIG. 1 shows an apparatus for removing CO from reformed gas according to a first embodiment of the present invention. 10
a, 10b, 10c... 10n are reactors, which are CO selective oxidation catalysts, for example Ru / Al ₂ O ₃ (A
Catalyst layer 12 of ruthenium-based catalyst using l ₂ O ₃ as carrier
a, 12b, 12c... 12n. The reactors 10a, 10b, 10c... 10n are provided in series and in multiple stages in the reformed gas conduit 14 through which the reformed gas containing CO flows, and the reformed gas at the outlet of each catalyst layer is cooled to be suitable for the reaction. A reformed gas temperature adjusting means 16 for adjusting the temperature is provided in the reformed gas conduit 14, and these reformed gas temperature adjusting means 1 are provided.
An oxidizing agent distribution / supplying means 18 is provided in the reformed gas conduit 14 between the catalyst layer 6 and each of the catalyst layers 12a, 12b, 12c... 12n. As the oxidizing agent, any one of air, oxygen, oxygen-enriched air and the like or a mixed gas thereof is used. 20 is a mixer. These mixers are not always necessary, and the oxidizing agent may be supplied directly to the reformed gas conduit 14 and mixed therein. 22 is a methanol reformer, 24 is a CO poisoning fuel cell such as PEFC (Polymer Polymer Fuel Cell), PAFC (phosphoric acid fuel cell), and 26 is a refrigerant flow rate control for controlling a cooling medium such as air or water. A valve 28 is an oxidant flow control valve.
Note that the reformed gas temperature adjusting means at the inlet of the first catalyst layer 12a is not always necessary.

FIG. 2 shows an example of the reformed gas temperature adjusting means 16. In this example, the reformed gas temperature adjusting means 16
Comprises a cooler 30 and a temperature instruction controller (TIC) 32 for detecting the temperature of the reformed gas in the reformed gas conduit and controlling the refrigerant flow control valve 26. In the apparatus configured as described above, when the temperature of the reformed gas containing CO from the methanol reformer 22 is higher than the optimum reaction temperature, the reformed gas temperature adjusting means 16 adjusts the temperature to a temperature suitable for the CO selective oxidation reaction. While being cooled, the oxidizing agent is supplied by the oxidizing agent distributing / supplying means 18 so that the first catalyst layer 12a
Will be introduced. When the temperature of the reformed gas containing CO from the methanol reformer 22 is the optimum reaction temperature, the reformed gas is introduced into the first catalyst layer 12a without cooling.
After a part of CO in the reformed gas is removed in the first catalyst layer 12a, the same operation as described above is performed to introduce the reformed gas containing CO into the second catalyst layer 12b, CO inside
, And then the same operation as described above is performed to introduce the third catalyst layer 12c,..., The n-th catalyst layer 12n, so that CO in the reformed gas is almost completely removed. You.

FIG. 3 shows an example of a control mechanism in the apparatus for removing carbon monoxide in reformed gas of the present invention. The temperature of the reformed gas at the inlet of the reactor 10a is controlled by the flow rate of the cooling medium. That is, the flow rate of the cooling medium is detected by the refrigerant flow rate indicating controller 60, the reformed gas temperature is detected by the reformed gas temperature indicating controller 62, and the flow rate of the cooling medium is adjusted so that the reformed gas temperature becomes the set value. It is controlled by the flow control valve 26. Also, the oxidant flow rate controller 64 detects the oxidant flow rate,
The reformed gas flow rate controller 66 detects the reformed gas flow rate, and the CO concentration analyzer 68 detects the CO concentration in the reformed gas. From these detected values, the necessary oxidant can be supplied. The flow rate of the oxidant (air or oxygen) is controlled by the oxidant flow control valve 28. Further, the reaction temperature of the catalyst layer of the reactor is adjusted by controlling the flow rate of the cooling medium. That is, a refrigerant passage 70 is provided in the reactor 10a, and the flow rate of the refrigerant to be introduced into the refrigerant passage 70 is detected by the refrigerant flow instruction controller 72, and the temperature of the catalyst layer 12a is detected by the catalyst temperature instruction controller 74. Based on these detected values, the refrigerant flow control valve 76 is controlled so that the reaction temperature of the catalyst layer 12a of the reactor 10a becomes a set value.

The catalyst layer 12 of the reactor 10 may be a conventional packed layer of catalyst particles 34 as shown in FIG. 4, or may be a honeycomb shape. However, in the configuration shown in FIG. 4, since the cooling and heat radiation of the catalyst layer 10 are not sufficiently performed, as shown in FIG. 5, a dilution filling method in which the catalyst particles 34 and the heat transfer particles 36 are mixed and filled is used. Is preferred. As the heat transfer particles, particles having no catalytic activity such as glass beads and ceramics, and particles of metals having no catalytic activity and high thermal conductivity such as aluminum and stainless steel are used.

FIG. 14 shows the catalyst layer 40 before being divided into the catalyst layers 12 shown in FIG. 4, and shows a case where the catalyst layer length is L ₀ . The catalyst layer 12 in the present invention is obtained by dividing the catalyst layer 40 shown in FIG. 14, it is shorter than the catalyst layer length L _0. The catalyst layer 40 filled only with the catalyst particles 34 shown in FIG. 14 is not preferable because the temperature of the catalyst layer rises due to the exothermic reaction and exceeds the upper limit temperature of the reaction as shown by the broken line in FIG. The catalyst used was Ru / A.
This figure shows a case in which l ₂ O ₃ particles are used and the catalyst layer is filled to a catalyst layer length L ₀ = 36 mm. Therefore, it is conceivable to fill the catalyst particles 34 mixed with the heat transfer particles 36 as shown in FIG. In this case, the length L _N of the catalyst layer is L ₀ × N.
Here, N is the dilution ratio of the catalyst. Ru as a catalyst
/ Al ₂ O ₃ particles and glass beads are used as heat transfer particles at a dilution ratio N = 6.3, the catalyst layer length L _N = L ₀ × N = 36 × 6.3 = 230 mm became.
In this case, as shown by the solid line in FIG. 16, the temperature distribution in the catalyst layer rises due to the exothermic reaction, but falls below the reaction upper limit temperature.

FIG. 15 shows a conventional catalyst charging method shown in FIG.
As a result of measurement of the reaction rate in the catalyst dilution and filling method shown in FIG. 14, in the ordinary catalyst filling method shown in FIG. 14, the CO removal rate was 99.0% and the outlet CO concentration was 100 ppm (SV
= 50000 hr ^-1 , LV = 0.496 Nm / sec), FIG.
In the catalyst dilution and filling method shown in FIG. 5, the CO removal rate was 99.84.
%, And the outlet CO concentration was 16 ppm (SV = 50,000).
hr ⁻¹ , LV = 0.496 Nm / sec). When the flow rate was halved, the CO removal rate was 99.93% and the outlet CO concentration was 7 ppm (SV = 25000 hr ⁻¹ , LV = 0.248 Nm / se).
c). The CO concentration in the reformed gas at the inlet was 10,000 ppm. However, in the dilution filling method, even though the catalyst layer temperature is lower than the reaction upper limit temperature, it is close to the reaction upper limit temperature, so that the catalyst layer is multi-staged in order to more reliably and further improve the reaction rate. Need to be split.

The shape of the reactor 10 is shown in FIGS.
As shown in FIG. 7, a tubular body in which the cylindrical main body 42 is filled with the catalyst particles 34 can be used. 44 is a jacket for flowing a cooling medium to cool the catalyst layer. As shown in FIGS. 8 and 9, the reactor 10 may have a structure in which a plurality of small tubes 46 filled with the catalyst particles 34 are inserted into a cylindrical main body 42. in this case,
The cooling medium is configured to flow between the small tubes.
Further, as shown in FIGS. 10 and 11, the reactor 10 may be a plate type in which the catalyst particles 34 are filled between two plates 48, 48. 50 is a cooling medium passage, and 52 is a heat insulating layer. When a plate-type reactor is used as the CO removal reactor, the reformer (reformer) and the CO converter can be integrated with each other, so that the fuel cell power generator can be made more compact.

FIG. 12 shows an apparatus for removing CO in reformed gas according to a second embodiment of the present invention. In this embodiment, the catalyst layer of each stage is divided into a ruthenium-based catalyst layer 54 on the upstream side and a rhodium-based catalyst layer 56 on the downstream side, and a part of the CO in the reformed gas is separated by the ruthenium-based catalyst layer 54. After the removal, the reformed gas heated by the reaction heat is introduced into the adjacent rhodium-based catalyst layer 56 to remove CO in the reformed gas. In the present embodiment, there is an advantage that the reaction heat can be used efficiently. Other configurations are the same as those in the first embodiment.

FIG. 13 is a graph showing the effect of temperature and catalyst on the CO.H ₂ oxidation reaction rate.印 indicates the temperature of the Rh-based catalyst (specifically, Rh / Al ₂ O ₃ was used) −η
In the CO curve, ● marks indicate Ru-based catalysts (specifically, Ru / Al ₂
Temperature -ηCO curve of O ₃ was used), □ mark temperature -ItaH ₂ curve of Rh catalyst _{(Rh / Al 2 O 3)} , ■ mark Ru
₂ shows a temperature-ηH ₂ curve of a system catalyst (Ru / Al ₂ O ₃ ). The gas composition at the inlet of the catalyst layer (catalyst particle packed layer) was 8500 ppm of hydrogen, 900 ppm of carbon monoxide, and 800 ppm of oxygen in all cases, and SV was 20,000 hr ^-1 and LV was in any case. Also 0.2
It was 15 Nm / sec.

From FIG. 13, when a Ru-based catalyst is used,
It can be seen that the CO oxidation reaction rate is high and the hydrogen oxidation reaction rate is low at 60 to 100 ° C. Also, the optimum temperature range is narrow Rh
When a system catalyst is used, the CO oxidation reaction rate is high at 120 to 150 ° C., and the hydrogen oxidation reaction rate is low. Therefore, in the case of the second embodiment shown in FIG.
For a reformed gas containing 100 ° C. of CO (including a reformed gas obtained by changing a higher temperature reformed gas to 60 to 100 ° C.), a reaction for removing CO with a Ru-based catalyst is advanced. Thus, the optimum temperature condition of the Rh-based catalyst is 1
The temperature is raised to 20 to 150 ° C., and CO is further removed with a Rh-based catalyst, so that the reaction amounts of hydrogen and methane due to side reactions can be reduced.

[0022]

As described above, the present invention has the following effects. (1) The catalyst layer for the selectoxo reaction is divided into multiple stages, and the reformed gas temperature adjusting means is provided at the outlet of each stage, so that the temperature distribution range per stage can be maintained at the optimum condition. Therefore, the reaction attainment rate and the selectivity (CO removal rate) can be improved. (2) When the heat transfer particles are mixed and filled into the catalyst particles, the temperature rise and heat removal of the catalyst layer due to the exothermic reaction can be efficiently performed. (3) When the catalyst layer of each stage is divided into a ruthenium-based catalyst on the upstream side and a rhodium-based catalyst on the downstream side, it is possible to solve the problem that the heat removal cannot keep up with the heat generation, and to reduce the reformed gas temperature. , The amount of hydrogen reduction and the amount of methane generated can be reduced.

[Brief description of the drawings]

FIG. 1 shows C in a reformed gas according to a first embodiment of the present invention.
It is a flow sheet which shows an O removal device.

FIG. 2 is a flow sheet showing details around a first catalyst layer and a second catalyst layer in FIG. 1;

FIG. 3 is a flow sheet showing an example of a control mechanism in the apparatus of the present invention.

FIG. 4 is an explanatory sectional view showing an example of a catalyst layer in FIG. 1;

FIG. 5 is an explanatory sectional view showing another example of the catalyst layer in FIG. 1;

FIG. 6 is an explanatory longitudinal sectional view showing one example of the catalytic reactor in FIG. 1;

FIG. 7 is an explanatory cross-sectional view of the same.

8 is an explanatory longitudinal sectional view showing another example of the catalytic reactor in FIG. 1. FIG.

FIG. 9 is an explanatory cross-sectional view of the same.

FIG. 10 is an explanatory longitudinal sectional view showing still another example of the catalytic reactor in FIG. 1;

FIG. 11 is an explanatory cross-sectional view of the same.

FIG. 12 is a flow sheet showing an apparatus for removing CO in reformed gas according to a second embodiment of the present invention.

FIG. 13 is a graph showing the relationship between the temperature, the CO oxidation reaction rate, and the H ₂ oxidation reaction rate when a Ru-based catalyst and a Rh-based catalyst are used.

FIG. 14 is an explanatory sectional view showing a catalyst layer of a normal filling method for uniformly filling only catalyst particles.

FIG. 15 is an explanatory sectional view showing a catalyst layer of a dilution and filling system of a catalyst in which catalyst particles and heat transfer particles are mixed.

FIG. 16 shows a catalyst layer of a normal filling type shown in FIG. 14 and FIG.
6 is a graph showing the relationship between the catalyst layer length and the catalyst layer reaction temperature in the catalyst layer of the dilution filling method shown in FIG.

[Explanation of symbols]

 10, 10a, 10b, 10c ... 10n Reactor 12, 12a, 12b, 12c ... 12n Catalyst layer 14 Reformed gas conduit 16 Reformed gas temperature control means 18 Oxidant distribution / supply means 20 Mixer 22 Methanol reformer 24 Fuel cell 26 , 76 Refrigerant flow control valve 28 Oxidant flow control valve 30 Cooler 32 Temperature indicator controller 34 Catalyst particles 36 Heat transfer particles 40 Catalyst layer 42 Cylindrical main body 44 Jacket 46 Small pipe 48 Plate 50 Cooling medium passage 52 Thermal insulation layer 54 Ruthenium system Catalyst layer 56 Rhodium-based catalyst layer 60, 72 Refrigerant flow rate indicator controller 62 Reformed gas temperature indicator controller 64 Oxidant flow rate indicator controller 66 Reformed gas flow rate indicator controller 68 CO concentration analyzer 70 Refrigerant passage 74 Catalyst temperature indicator Controller

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁶ Identification code Agency reference number FI Technical indication location H01M 8/04 C01B 31/18 B // C01B 31/18 B01D 53/36 Z (72) Inventor Ikuo Nagashima 1-1, Kawasaki-cho, Akashi-shi, Hyogo Prefecture Inside the Akashi factory of Kawasaki Heavy Industries, Ltd. (72) Inventor Seiji Terada 1-1-1, Kawasaki-cho, Akashi-shi, Hyogo Kawasaki Heavy Industries, Ltd.

Claims (12)

[Claims] 1. A method for sequentially supplying a reformed gas containing carbon monoxide to a carbon monoxide selective oxidation catalyst layer provided in multiple stages in a gas flow direction, wherein a reformed gas at an outlet of each catalyst layer is provided. A method for cooling carbon monoxide to a temperature suitable for the reaction and distributing and supplying an oxidizing agent to each catalyst layer. 2. The method for removing carbon monoxide in a reformed gas according to claim 1, wherein a ruthenium-based catalyst is used as a carbon monoxide selective oxidation catalyst, and the temperature of each catalyst layer is maintained in a range of 60 to 210 ° C. 3. The method for removing carbon monoxide in a reformed gas according to claim 1, wherein a rhodium-based catalyst is used as a carbon monoxide selective oxidation catalyst, and the temperature of each catalyst layer is maintained in a range of 130 to 210 ° C. 4. The catalyst layer of each stage is divided into a ruthenium-based catalyst layer and a rhodium-based catalyst layer, and the reformed gas is treated with the ruthenium-based catalyst layer. The method for removing carbon monoxide in a reformed gas according to claim 1, wherein the treatment is performed with a catalyst layer. 5. The temperature of the reformed gas introduced into the ruthenium-based catalyst layer is in the range of 60 to 100 ° C., and the temperature of the reformed gas introduced into the adjacent rhodium-based catalyst layer is 120 to 150 ° C.
5. The method for removing carbon monoxide in a reformed gas according to claim 4, wherein: 6. The reformed gas according to claim 1, wherein the oxidizing agent is distributed and supplied such that the O ₂ / CO molar ratio at each catalyst layer inlet is in the range of 0.5 to 1.5. Carbon monoxide removal method. 7. The reformed gas according to claim 1, wherein catalyst particles are used as the catalyst, and at least one of glass beads, ceramic particles, and metal particles is mixed with the catalyst particles. Carbon oxide removal method. 8. Reactors provided with a catalyst layer of a carbon monoxide selective oxidation catalyst are provided in multiple stages in a reformed gas conduit through which a reformed gas containing carbon monoxide flows, and a reformed gas at an outlet of each catalyst layer is provided. A reformed gas temperature adjusting means for cooling and adjusting to a temperature suitable for the reaction is provided in the reformed gas conduit, and the oxidizing agent is distributed to the reformed gas conduit between the reformed gas temperature adjusting means and each catalyst layer. An apparatus for removing carbon monoxide in a reformed gas, comprising a supply unit. 9. The apparatus for removing carbon monoxide in a reformed gas according to claim 8, wherein each catalyst layer is divided into a ruthenium-based catalyst layer on the upstream side and a rhodium-based catalyst layer on the downstream side. 10. The apparatus for removing carbon monoxide in a reformed gas according to claim 8, wherein the reactor has a tubular shape in which a cylindrical body is filled with a catalyst. 11. The apparatus for removing carbon monoxide in a reformed gas according to claim 8, wherein the reactor is a plate type in which a catalyst is filled between two plates. 12. The reactor in which a plurality of small tubes filled with a catalyst are inserted into a cylindrical main body.
An apparatus for removing carbon monoxide in a reformed gas as described in the above.