JPH059362B2 - - Google Patents

Info

Publication number
JPH059362B2
JPH059362B2 JP22859484A JP22859484A JPH059362B2 JP H059362 B2 JPH059362 B2 JP H059362B2 JP 22859484 A JP22859484 A JP 22859484A JP 22859484 A JP22859484 A JP 22859484A JP H059362 B2 JPH059362 B2 JP H059362B2
Authority
JP
Japan
Prior art keywords
combustion
catalyst
reaction
heat transfer
section
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
JP22859484A
Other languages
Japanese (ja)
Other versions
JPS61106402A (en
Inventor
Tetsuro Okano
Kengo Uematsu
Naruhito Takamoto
Hiroyuki Kako
Hiroshi Ishizaka
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Mitsubishi Power Ltd
Original Assignee
Babcock Hitachi KK
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Babcock Hitachi KK filed Critical Babcock Hitachi KK
Priority to JP22859484A priority Critical patent/JPS61106402A/en
Publication of JPS61106402A publication Critical patent/JPS61106402A/en
Publication of JPH059362B2 publication Critical patent/JPH059362B2/ja
Granted legal-status Critical Current

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Classifications

    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0446Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
    • B01J8/0449Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical beds
    • B01J8/0453Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical beds the beds being superimposed one above the other
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/0285Heating or cooling the reactor
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008Controlling the process
    • B01J2208/00017Controlling the temperature
    • B01J2208/00106Controlling the temperature by indirect heat exchange
    • B01J2208/00115Controlling the temperature by indirect heat exchange with heat exchange elements inside the bed of solid particles
    • B01J2208/00132Tubes

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Description

【発明の詳細な説明】[Detailed description of the invention]

(産業上の利用分野) 本発明は触媒燃焼式反応器におよびその燃焼方
法に係り、特にホツトスポツト防止と、効率的な
伝熱を可能にした触媒燃焼式反応器およびその燃
焼方法に関するものである。 (従来の技術) 燃料電池用改質器(以下、改質器をリフオーマ
と称することがある)は、例えばリン酸燃料電池
システムにおいて、電池に必要な水素(H2)を
天然ガス等を原料にして製造する装置であり、改
質触媒層に通した天然ガス(主成分はCH4であ
り、以下CH4と記すことがある)と水蒸気を反応
部で加熱してH2を得るものである。 CH4+H2O→3H2+CO 第14図は、燃料電池およびこれに付ずいする
改質ガス製造装置の系統図を示したもので、反応
管部1Aおよび燃焼部1Bとを有するリフオーマ
1と、高温および低温シフトコンバータ3および
2と、燃料電池のアノード5およびカソード6
と、コンプレツサ7およびタービン8、およびこ
れらの関連配管類からなつている。 燃料電池への要求性能の中で重要なものは、小
型高効率、低公害であり、このような要求性能は
燃焼部を有するリフオーマの性能にかかつてく
る。この性能を満足するために、燃焼部に燃焼触
媒を用いた触媒燃焼式リフオーマが注目されてい
る。燃焼触媒を用いると、燃焼部(触媒充填層)
において、充填層伝熱による高い伝熱係数が得ら
れ、NOxの発生もほとんどなく、前述の要求性
能を満足させることができる。 (発明が解決しようとする問題点) しかし、触媒充填式リフオーマにおいては、下
記の問題点があることがわかつた。すなわち、燃
焼触媒は活性が高く、燃料は触媒表面で燃焼し
て、高温を発生するが、現状技術では、触媒寿命
が短いため、すぐに活性を失つてしまう。また燃
料は供給された部分で主に燃焼するため、反応部
が不均一加熱されて反応にムラが生ずる可能性が
ある。 この対策として、現在は空気と燃料を空気過剰
の状態に混合した後、燃焼触媒層に供給する触媒
バーナ方式がとられている。第13図は、従来の
触媒バーナ式リフオーマの概念図である。原料の
CH4とH2Oはノズル11から供給され、改質触媒
層12に入る。ここで伝熱粒子の充填された燃焼
部(充填部)から熱を受けとつて反応を起こし、
H2リツチの改質ガスとなる。この改質ガスは反
応管内管14を通り、原料ガスと熱交換を行ない
ながら、ノズル21から系外にとり出される。一
方、充填部ではノズル15から供給された燃料の
アノード廃ガスとノズル16から供給された空気
が予混合層17で混合したのち燃焼触媒層18で
燃焼し、燃焼ガスは伝熱粒子層19で反応部に熱
を与えた後、ノズル20から系外に排出される。 しかし、上記触媒バーナ方式においては、理論
燃焼温度を触媒の耐熱温度以下に設定し、燃焼を
1回で行なわせているため、空気が大過剰の状態
となり、燃焼ガス持出し顕熱が増加し、熱効率が
低下するという欠点がある。 また反応部の温度制御法は、反応管の管壁温度
と、反応部の出口ガス温度を測定し、反応管の安
全温度と改質ガスの出口温度で制御をしている
が、このような制御法では急激な負荷変動に対し
て応答性が充分でないという欠点がある。 本発明の目的は、触媒燃焼層におけるホツトス
ポツトの発生を防止し、熱効率の低下を改善し、
効果的な伝熱を可能にする触媒燃焼式反応器およ
びその燃焼方法を提供することにある。 (問題点を解決するための手段) 本発明は、触媒および伝熱粒子を充填した反応
器に反応管を挿入し、該触媒および伝熱粒子の充
填部に燃料ガスを供給して燃焼させ、前記反応管
を加熱して該管内を通る原料を分解、改質する装
置において、前記反応管の下部と反応部の位置の
触媒および伝熱粒子充填部の少なくとも2個所に
燃料ガスを供給する手段を設け、少なくとも前記
反応部に相当する充填部の粒子径を他の部分のそ
れよりも大にしたことを特徴とするものである。 また本発明の燃焼方法は、触媒および伝熱粒子
を層状に充填した反応器に反応管を挿入し、該反
応管の下部と反応部の位置の触媒充填層の少なく
とも2個所に燃料ガスを供給して燃焼させ、前記
反応管を加熱して該管内を通る原料を分解、改質
する触媒燃焼式反応器の燃焼方法において、前記
反応管の反応部に相当する触媒充填層に供給する
燃料ガスを一旦触媒充填層の下層の伝熱粒子層に
供給し、該燃焼ガスを充填層全体に広げた後、前
記触媒充填層に流入させることを特徴とするもの
である。 以下、本発明を図面によりさらに詳細に説明す
る。 (実施例) 第1図は、本発明の一実施例を示す触媒燃焼式
リフオーマの概略図である。この装置は、反応器
31内に設けられた反応管34およびその内管4
3と、該反応管34のまわりに充填された燃焼用
触媒42と、燃料ガスの供給口32および41
と、燃焼用の空気供給口33と、原料ガスの入口
36および生成ガスの出口37と、燃焼排ガスの
出口35とから主として構成される。図におい
て、燃料ガスは反応器の充填層下部から供給され
る一方、さらに塔中央部のガス供給口41からも
同時に供給される。該供給口32および41から
供給された燃料ガスは、最初に大粒径触媒42の
部分で燃焼して高温ガスを発生し、高温ゾーン4
0を形成する。この付近では反応管34への伝熱
は輻射伝熱が支配的となるため、できるかぎり大
粒径の触媒を充填することが好ましい。一方、原
料ガスであるメタンとスチームは原料入口36か
ら反応管内に供給され、700℃の温度になると改
質反応により水素リツチガスを生成する。生成し
た水素リツチガスは反応管の内管43を通つて生
成ガス出口37から系外に取出される。 燃焼ガスは反応器の上部に行くにつれて反応管
に熱を奪われて温度が低下し、低温ゾーン39で
は通常の触媒粒子38との接触により効率よく熱
を反応器34に伝え、燃焼排ガスとして出口35
から系外に排出される。なお、第1−A図および
第1−B図に、塔中央部の燃料ガス供給法の例を
示したが、第1−A図では燃料を反応器に対して
直角に供給する場合、および第1−B図では接線
方向に供給する場合をそれぞれ示す。いずれの場
合も供給口が4個所のケースを示したが、これは
1個所または2個所以上設けてもよく、さらに塔
の高さ方向に2段以上供給口を設置することも可
能である。 第2図は、第1図において塔中央部の燃料供給
口を設けずに、塔底部からのみ燃料ガスを供給す
る従来の触媒燃焼式反応装置と本発明の反応装置
の反応管表面温度分布を比較して示した図であ
る。この場合、原料ガスと燃料ガスは同じ量を供
給した場合を比較しているが、本発明Aでは従来
法Bに比べ、700℃以上の改質ゾーンの反応管長
さが長く、しかも均一になつていることがわか
る。これより本発明のほうが、部分的なヒートス
ポツトが生じにくく、改質反応が円滑に行なわれ
ることが理解される。また700℃以下の低温ゾー
ンでは、通常の小さい触媒粒子との対流伝熱によ
り容易に燃焼廃ガスの熱交換が行なわれるため、
このゾーンにおける反応管長さを短くすることが
可能となる。 第1図の実施例において、反応塔内に充填する
触媒粒子は、燃料ガスを供給する部分以外の触媒
粒子径は2〜7mmであるが、燃料ガスの供給口付
近の触媒粒子径はその2倍以上の大きさの粒子を
充填することが好ましい。その理由としては、第
3図に示すように触媒充填層内の総括伝熱係数は
1000℃以上の高温域では対流よりも輻射が支配的
となり、このため吸熱反応が起こる高温域では触
媒粒子径を大きくし、輻射伝熱係数を上げること
が望ましい(第3図の触媒粒子径5mm、ガス通過
速度0.3m/s)。また第4図は、輻射伝熱係数に
及ぼす粒径の影響を示したものであるが、温度
800℃の場合には粒径を大きくしてもそれほど輻
射伝熱係数は大きくならないが、1200℃の場合に
は粒径を10mmにすると5mmの2倍以上になり、粒
径を大きくすることによつて輻射伝熱係数を高め
ることが明らかである(第4図のガス通過速度
0.3m/s)。 上記実施例によれば、触媒充填層型のリフオー
マにおいて、燃料ガスを反応器の充填層下部と中
央部の少なくとも2個所から供給し、かつ燃料供
給部の触媒層の粒子径を大きくすることにより、
改質反応ゾーンの伝熱効果を高め、反応管温度を
均一にすることができる。 第1図の実施例では、反応器の下部と中央部に
供給する燃料ガスは同一のものとして説明した
が、反応管内の反応特性を応じて異なる燃料ガス
を供給することができ、また反応管のまわりの触
媒充填部は、必要に応じて燃焼活性のない伝熱粒
子の充填部を設けることができる。特に後述する
ように反応部に供給する燃焼ガスは伝熱粒子層を
通して拡散させた後、触媒粒子層を通した方が局
部的温度上昇を防止することができる。 第5図は、反応器の下部と中央部とにそれぞれ
反応特性に応じて異なる燃料ガスを供給した実施
例を示すもので、反応器の下部に燃料電池のアノ
ード廃ガスを、中央部に天然ガス(主として
CH4)を供給し、反応器中央部の燃料(CH4)を
供給する部分には伝熱粒子の充填のみとし、か
つ、この伝熱粒子の充填部はCH4が拡散しやすい
ように他の部分よりも大きい径の充填粒子を用い
たものである。 すなわち、第5図の実施例は、反応器の2個所
に供給される燃料を異なる種類のものとし、これ
らの燃焼特性の相違を利用して反応管の加熱部に
おけるホツトスポツトの発生を防止し、また同一
燃料を用いた場合の空気大過剰により熱効率の低
下を改善し、効果的な伝熱を図つたものである。 反応器に供給する燃料としては、燃料電池のア
ノードからリサイクルされるアノード廃ガス(水
素を主体とする)と助燃用の天然ガス(以下、
CH4で代表する)が好適に使用される。該アノー
ド廃ガスの主な燃焼成分はH2であるが、H2
CH4の燃焼特性には第1表に示すようにかなりの
相違がある。
(Industrial Application Field) The present invention relates to a catalytic combustion reactor and its combustion method, and particularly relates to a catalytic combustion reactor and its combustion method that enable hot spot prevention and efficient heat transfer. . (Prior art) A fuel cell reformer (hereinafter sometimes referred to as a reformer) is used, for example, in a phosphoric acid fuel cell system, to convert hydrogen (H 2 ) necessary for the battery from natural gas or other raw material. This is a device that produces H2 by heating natural gas (the main component is CH4 , hereinafter referred to as CH4 ) passed through a reforming catalyst bed and steam in a reaction section. be. CH 4 +H 2 O → 3H 2 +CO Figure 14 shows a system diagram of a fuel cell and a reformed gas production device attached thereto. , high and low temperature shift converters 3 and 2 and the anode 5 and cathode 6 of the fuel cell.
It consists of a compressor 7, a turbine 8, and their related piping. The important performance requirements for a fuel cell are small size, high efficiency, and low pollution, and these performance requirements are related to the performance of a rifoma that has a combustion section. In order to satisfy this performance, catalytic combustion type refurmers that use a combustion catalyst in the combustion section are attracting attention. When a combustion catalyst is used, the combustion part (catalyst packed bed)
In this method, a high heat transfer coefficient is obtained due to packed bed heat transfer, almost no NOx is generated, and the above-mentioned required performance can be satisfied. (Problems to be Solved by the Invention) However, it has been found that the catalyst-filled reformer has the following problems. That is, combustion catalysts have high activity, and fuel burns on the surface of the catalyst to generate high temperatures, but with current technology, the catalyst life is short and the catalyst quickly loses its activity. Furthermore, since the fuel is mainly combusted in the portion where it is supplied, there is a possibility that the reaction portion may be heated unevenly, resulting in uneven reaction. As a countermeasure to this problem, a catalytic burner system is currently used in which air and fuel are mixed in an excess air state and then supplied to the combustion catalyst layer. FIG. 13 is a conceptual diagram of a conventional catalytic burner type reheater. of raw materials
CH 4 and H 2 O are supplied from the nozzle 11 and enter the reforming catalyst layer 12 . Here, heat is received from the combustion part (filling part) filled with heat transfer particles to cause a reaction.
It becomes a reformed gas rich in H2 . This reformed gas passes through the reaction tube inner tube 14 and is taken out of the system from the nozzle 21 while exchanging heat with the raw material gas. On the other hand, in the filling section, the anode waste gas of the fuel supplied from the nozzle 15 and the air supplied from the nozzle 16 are mixed in the premixing layer 17 and then combusted in the combustion catalyst layer 18, and the combustion gas is transferred to the heat transfer particle layer 19. After applying heat to the reaction section, it is discharged from the nozzle 20 to the outside of the system. However, in the above-mentioned catalytic burner method, the theoretical combustion temperature is set below the heat-resistant temperature of the catalyst and combustion is performed in one go, resulting in a large excess of air and an increase in the sensible heat carried out by the combustion gas. The disadvantage is that thermal efficiency decreases. In addition, the temperature control method for the reaction section measures the tube wall temperature of the reaction tube and the outlet gas temperature of the reaction section, and controls based on the safe temperature of the reaction tube and the exit temperature of the reformed gas. The control method has the disadvantage that it does not have sufficient responsiveness to sudden load changes. The purpose of the present invention is to prevent the occurrence of hot spots in the catalytic combustion layer, improve the reduction in thermal efficiency,
An object of the present invention is to provide a catalytic combustion reactor that enables effective heat transfer and a combustion method thereof. (Means for Solving the Problems) The present invention includes inserting a reaction tube into a reactor filled with a catalyst and heat transfer particles, supplying fuel gas to the portion filled with the catalyst and heat transfer particles to cause combustion, In an apparatus for heating the reaction tube to decompose and reform the raw material passing through the tube, means for supplying fuel gas to at least two locations: the lower part of the reaction tube and the catalyst and heat transfer particle filling section located at the reaction section. The present invention is characterized in that the particle size of at least the packed portion corresponding to the reaction portion is larger than that of the other portions. Furthermore, in the combustion method of the present invention, a reaction tube is inserted into a reactor filled with a catalyst and heat transfer particles in a layered manner, and fuel gas is supplied to at least two locations: the lower part of the reaction tube and the catalyst packed bed at the reaction section. In a combustion method for a catalytic combustion reactor in which the raw material passing through the tube is decomposed and reformed by heating the reaction tube and burning the fuel gas, the fuel gas is supplied to a catalyst packed bed corresponding to the reaction section of the reaction tube. The method is characterized in that the combustion gas is once supplied to the heat transfer particle layer below the catalyst packed bed, and after the combustion gas is spread over the entire packed bed, it is made to flow into the catalyst packed bed. Hereinafter, the present invention will be explained in more detail with reference to the drawings. (Example) FIG. 1 is a schematic diagram of a catalytic combustion type re-former showing an example of the present invention. This device includes a reaction tube 34 provided in a reactor 31 and an inner tube 4 thereof.
3, a combustion catalyst 42 filled around the reaction tube 34, and fuel gas supply ports 32 and 41.
, an air supply port 33 for combustion, an inlet 36 for raw material gas, an outlet 37 for generated gas, and an outlet 35 for combustion exhaust gas. In the figure, while fuel gas is supplied from the lower part of the packed bed of the reactor, it is also simultaneously supplied from the gas supply port 41 in the center of the column. The fuel gas supplied from the supply ports 32 and 41 is first combusted at the large particle size catalyst 42 to generate high temperature gas, and is then transferred to the high temperature zone 4.
form 0. In this vicinity, heat transfer to the reaction tube 34 is dominated by radiation heat transfer, so it is preferable to fill the catalyst with a particle size as large as possible. On the other hand, methane and steam, which are raw material gases, are supplied into the reaction tube from the raw material inlet 36, and when the temperature reaches 700° C., hydrogen-rich gas is produced by a reforming reaction. The generated hydrogen-rich gas is taken out of the system from the generated gas outlet 37 through the inner tube 43 of the reaction tube. As the combustion gas goes to the top of the reactor, heat is taken away by the reaction tube and the temperature decreases, and in the low temperature zone 39, the heat is efficiently transferred to the reactor 34 by contact with the normal catalyst particles 38, and it exits as combustion exhaust gas. 35
is discharged from the system. Note that Fig. 1-A and Fig. 1-B show an example of a method for supplying fuel gas to the center of the column, but Fig. 1-A shows cases in which fuel is supplied perpendicularly to the reactor, and FIG. 1-B shows the case of feeding in the tangential direction. In each case, a case is shown in which there are four supply ports, but one or more supply ports may be provided, and it is also possible to provide two or more supply ports in the height direction of the tower. Figure 2 shows the reaction tube surface temperature distribution of a conventional catalytic combustion reactor that supplies fuel gas only from the bottom of the tower without providing a fuel supply port in the center of the tower in Figure 1, and the reactor of the present invention. It is a diagram shown in comparison. In this case, the case where the same amount of raw material gas and fuel gas are supplied is compared, but in Invention A, the length of the reaction tube in the reforming zone of 700°C or higher is longer and more uniform than in Conventional Method B. You can see that From this, it is understood that in the present invention, local heat spots are less likely to occur and the reforming reaction is carried out more smoothly. In addition, in the low temperature zone below 700℃, heat exchange of combustion waste gas is easily carried out through convective heat transfer with ordinary small catalyst particles.
It becomes possible to shorten the length of the reaction tube in this zone. In the embodiment shown in Fig. 1, the diameter of the catalyst particles packed in the reaction tower is 2 to 7 mm in areas other than the part where the fuel gas is supplied, but the diameter of the catalyst particles near the fuel gas supply port is 2 to 7 mm. It is preferable to fill the particles with particles that are twice the size or more. The reason for this is that, as shown in Figure 3, the overall heat transfer coefficient in the catalyst packed bed is
In the high temperature range of 1000°C or higher, radiation becomes more dominant than convection. Therefore, in the high temperature range where endothermic reactions occur, it is desirable to increase the catalyst particle size and increase the radiation heat transfer coefficient (catalyst particle size 5 mm in Figure 3). , gas passing speed 0.3 m/s). Figure 4 shows the effect of particle size on the radiant heat transfer coefficient.
At 800℃, the radiation heat transfer coefficient does not increase much even if the particle size is increased, but at 1200℃, increasing the particle size to 10mm increases it to more than twice that of 5mm, which makes it difficult to increase the particle size. Therefore, it is clear that the radiation heat transfer coefficient is increased (gas passage velocity in Figure 4).
0.3m/s). According to the above embodiment, in the catalyst-packed bed type re-former, fuel gas is supplied from at least two locations in the reactor, one at the bottom of the packed bed and the other at the center, and the particle size of the catalyst layer in the fuel supply section is increased. ,
The heat transfer effect in the reforming reaction zone can be enhanced and the reaction tube temperature can be made uniform. In the embodiment shown in Fig. 1, the same fuel gas is supplied to the lower part and the center of the reactor, but it is possible to supply different fuel gases depending on the reaction characteristics inside the reaction tube. The surrounding catalyst filling portion may be provided with a filling portion of heat transfer particles having no combustion activity, if necessary. Particularly, as will be described later, if the combustion gas supplied to the reaction section is diffused through the heat transfer particle layer and then passed through the catalyst particle layer, local temperature increases can be prevented. Figure 5 shows an example in which different fuel gases were supplied to the lower part and center of the reactor depending on the reaction characteristics, with fuel cell anode waste gas being supplied to the lower part of the reactor and natural gas (mainly
CH 4 ) is supplied, and the fuel (CH 4 ) supplying part in the center of the reactor is filled only with heat transfer particles. This uses filled particles with a diameter larger than that of the part. That is, in the embodiment shown in FIG. 5, different types of fuel are supplied to two locations in the reactor, and the difference in combustion characteristics of these fuels is utilized to prevent the occurrence of hot spots in the heating section of the reaction tube. In addition, the reduction in thermal efficiency caused by a large excess of air when using the same fuel is improved, and effective heat transfer is achieved. The fuel supplied to the reactor is anode waste gas (mainly hydrogen) recycled from the fuel cell anode and natural gas for auxiliary combustion (hereinafter referred to as
CH 4 ) is preferably used. The main combustion component of the anode waste gas is H2 , but H2 and
There are considerable differences in the combustion characteristics of CH 4 as shown in Table 1.

【表】 第1表から明らかなように、H2は着火に要す
るエネルギーがCH4の1/10と小さく、触媒を用い
れば常温近くでも着火が可能であり、また燃焼速
度についても気体中で最も早く、さらに燃焼に必
要な空気量も最も少ない。これに対し、CH4は着
火温度が高く、燃焼速度が遅く、また燃焼に必要
な空気量もH2の3倍である。 本発明者らは、上記の2種の燃料を用い、第5
図に示すような触媒バーナ式リフオーマを用いて
種々の実験を行なつた、その結果次のことが明ら
かになつた。 (1) 空気量一定で、H2量のみを増加(空気に対
するH2濃度1.2→1.5%)すると、触媒バーナ部
のみ温度が上昇した(第6図参照)。図中、C
はH2量小、DはH2量大の場合を示す。 (2) 空気量一定で、CH4量のみを増加(空気に対
するCH4濃度1.5%→2.3%)すると、触媒バー
ナ部の温度はあまり上がらず、最高温度部は伝
熱粒子層に移動した(第7図参照)。図中、E
はCH4量小、FはCH4最大の場合を示す。 (3) 燃焼用空気量を加減して燃焼部流速を増加
(燃焼部空塔速度約0.2m/s→0.3m/s)さ
せたところ、流速の増加するに伴い、最高温度
域は上昇する傾向を示した(第8図参照)。図
中、Gは流速(空気量)小、Hは流速大の場合
を示す。また、反応部は吸熱反応であるが、吸
熱量の分布を調べたところ、反応部温度が650
〜700℃の位置で最も大きな吸熱量を示し、ヒ
ートフラツクスが大きくなることがわかつた。 以上の結果より、従来は燃料を直接触媒層に供
給するとホツトスポツトを生ずると考えられてき
たが、これは燃焼速度の速いH2の燃焼が原因で
あり、CH4は完全に燃焼するまでに時間がかか
り、充填層に拡散した後、燃焼することがわかつ
た。 なお、従来のリフオーマの燃焼ガスは反応部の
ガスと対向流に流されるが、反応部の出口温度は
750〜800℃であるため、著しい吸熱ゾーンを形成
する650〜700℃の範囲から出口温度まで顕熱上昇
があり、燃焼ガスの顕熱がこの顕熱上昇に使われ
るため、(650〜700℃)の吸熱ゾーンでは燃焼ガ
ス温度が低下し、反応部との間に充分な温度差が
大きくとれなくなり、従つて伝熱面を増加しなけ
ればならないことがわかつた。 第5図に示したリフオーマは、反応管の吸熱部
(反応部)に相当する燃焼部(充填部)に高カロ
リー燃料ガス(例えば天然ガス、CH4)の供給管
15Aを設け、また燃焼部の充填層を下から順に
燃焼触媒第1層18A、伝熱粒子層第1層19
A、伝熱粒子層第2層19B、燃焼触媒第2層1
8B、伝熱粒子層第3層19Cおよび金属粒子層
19Mとし、反応器底部の低カロリー燃料ガス供
給管15からアノード廃ガス(水素ガス)を供給
し、上部の高カロリー燃料の供給管15Aから天
然ガス(CH4)を供給するようにした点で第13
図の従来装置と異なつている。 このような構成の装置において、燃焼速度の速
いH2はガス供給管15から燃料、空気予混合ゾ
ーン17に導入され、ここで空気供給管16から
供給される空気とともに混合し、燃焼触媒第1層
(触媒バーナ)18Aに入り、ここで燃焼され、
その燃焼熱は反応管14にの先端部の伝熱に用い
られる。反応管14の先端部での伝熱は、主に吸
熱部ゾーンを過ぎた反応部流体の顕熱上昇用に用
いられる。燃焼触媒第1層18Aの燃焼ガスは伝
熱粒子層第1層19Aで反応管の反応部に熱を与
えて温度が低下する。この温度低下した燃焼ガス
は、次に吸熱ゾーンに入り、反応管中央部の燃料
供給管15Aから供給される高カロリー燃料の燃
焼熱によつて加熱される。すなわち、反応管の反
応部(吸熱ゾーン)の加熱には、燃料供給管15
Aから供給される、燃焼速度の遅いCH4が用いら
れる。このCH4が供給される部分には、燃焼活性
のない伝熱粒子の充填層(伝熱粒子層第2層19
B)が充填されているため、その上流側の燃焼触
媒部で完全燃焼される前に充填部内に充分に拡散
される。この伝熱粒子層第2層19Bの充填物は
CH4が拡散しやすいように径を大きめにしておく
ことが好ましい。このようにして充填部に拡散し
たCH4は、その下流側の燃焼触媒第2層18Bに
入り、一挙に燃焼する。燃焼触媒第2層の位置
は、通常運転時に反応部温度が650℃前後になる
ように設定される。該燃焼触媒第2層18Bの上
にはさらに伝熱粒子層第3層が設けられ、さらに
その上には金属粒子層19Mが設けられている。
この金属粒子層19Mに切り替える位置は、燃焼
ガス温度が700℃程度にまで低下する点が好まし
い。金属粒子層19Mの金属粒子は、アルミナ等
の耐火物からなる伝熱粒子層19Cよりも耐熱性
が低く、また重量の増加にもつながるが、第9図
に示すように熱伝導率が大きいため、伝熱係数を
向上させることができる。また、金属粒子は密度
が大きいため、流速増大時に軽い耐火物粒子が飛
散するのを防止する効果もある。 なお、充填層の伝熱係数は輻射の大きい高温域
において、粒子径の大きいほど大きな値を示す。
従つて反応器下部の伝熱粒子層19Aおよび19
Bの粒子は、上部の伝熱粒子層19Cの粒子より
径を大きくすることが好ましい。 次に第10図および第11図を用いて上記触媒
燃焼反応器の反応部および燃焼部の温度制御につ
いて説明する。 反応塔内の温度を測定する熱電対は、反応管の
軸方向に等間隔に複数個(この場合はA,B,
C,DおよびEの5個)取り付けられ、またその
まわりの燃焼部(充填部)にも反応部と同じ高さ
に熱電対A′,B′,C′,D′およびE′が取り付けら
れ、さらに反応管保護用の熱電対Fが反応管戻り
部の反応管表面に取り付けられている。上記熱電
対C,Dの間に反応部の吸熱ゾーンが来るように
設計時に各寸法を決定しておき、また燃料供給管
15Aは熱電対Dとほぼ同じ高さとなるように配
置する。空気供給管16には空気流量調節弁47
が、上段および下段の燃料供給管15Aおよび1
5にはそれぞれ天然ガス(CH4)流量調節弁48
および下段天然ガス流量調節弁49がそれぞれ設
けられ、これらは前記空気流量調節弁47に電気
的に接続される前記各熱電対の電気回路にそれぞ
れ接続されている。 このような構成において、燃料および空気の制
御法は下記のとおりである。まずA〜Eの熱電対
の指示値を読み、計算機の中に反応部の温度プロ
フイルを書かせる。次にA′〜D′の熱電対の指示
値を読み、燃焼部の温度プロフイルを計算機の中
に書かせる。次に双方の温度プロフイルを重ね、
反応部の吸熱ゾーンとCH4燃焼による燃焼温度の
極大部分が重なるようにCH4バルブ48,49お
よび空気バルブ47を調整する。この際の空気量
は、第1段目および第2段目の燃焼触媒層18A
および18Bの理論燃焼温度が触媒の耐熱限界温
度を超えず、かつ過剰空気率をできるだけ抑える
量を前もつて算出しておき、CH4の供給量に伴
い、適量の空気をバルブ47によつて供給する。
燃焼部の温度極大部分の上昇および下降はバルブ
48および49を用いて行なう。すなわち極大部
分を上昇させる場合にはバルブ49を閉じ、バル
ブ48を開き、一方下降させる場合にはバルブ4
9を開き、バルブ48を閉じる。また負荷変動運
転時には、吸熱ゾーンは熱電対CおよびDの間か
ら離れる場合があるが、燃焼部の制御は同様にバ
ルブ48と49の開閉によつて行なう。このよう
な2段燃焼の温度制御コントロールにより、熱の
必要な吸熱ゾーンに大量の熱を効果的に与えるこ
とができ、伝熱面積を最小にすることができる。 第12図は、計算機の具体的な制御プログラム
の一例を示したものである。このうち、吸熱ゾー
ンの判別は、A〜Eの熱電対の指示値のうちで、
650℃と700℃の両側の値を検出し、両者にはさま
れた空間を吸熱ゾーンとする。例えばCが620℃、
Dが710℃の場合、CDにはさまれた区間3を吸熱
ゾーンとする。また燃焼ゾーンの温度極大値Tp
の判明は、E′を除くA′〜D′で温度の最大値を判
別し、温度極大値Tpとする。例えばC′が最大値
の場合、C′がTpとなる。次にTpが吸熱ゾーンよ
り下にあるか否かの判別は、この場合はC′がTp
であるので、Tpは吸熱ゾーンより上にある。操
作はバルブ48をしぼり、バルブ49を開く。こ
れにより触媒バーナ(第1段燃焼触媒)側が加熱
されることになり、Tpは下降する。管璧温度F
の設定値は反応管の設計温度をもとに決定され
る。このプログラムは適当な間隔(例えば1分)
をもつて繰返す無限ループとする。例えば次の時
刻にTpがD′まで下降した場合、今度はバルブ4
8を開き、バルブ49がしぼられ、Tpは上昇す
る。すなわちTpは吸熱ゾーンの上端と下端の間
をゆつくり往復することになる。 上記実施例によれば、反応部の吸熱ゾーンを効
果的に加熱することにより、従来型リフオーマよ
り伝熱面積を例えば20〜40%小さくすることがで
き、また燃焼用空気量を抑えることができるた
め、排ガス持出し顕熱が減少し、熱効率が例えば
10〜20%向上する。さらに反応部および燃焼部の
温度プロフイルによる制御によつていかなる負荷
状態においても高効率運転が可能になる。 (発明の効果) 本発明によれば、触媒充填型のリフオーマにお
いて、燃料ガスを反応器の充填層下部とその上部
の少なくとも2個所から供給し、かつ燃料供給部
の充填粒子の径を大きくすることにより、伝熱性
能を高め、かつ改質反応ゾーンの反応管温度を均
一することができ、また上記2個所の燃料供給部
から、例えばそれぞれ低カロリーおよび高カロリ
ー燃料を供給し、また触媒充填層を燃焼触媒層と
伝熱粒子層を交互に設けることにより、改質反応
ゾーンすなわち吸熱ゾーンを効果的に加熱し、伝
熱面積を小さくすることができ、また燃焼用空気
量を少なくし、排ガス持出し顕熱を減少させ、熱
効率を向上させることができる。
[Table] As is clear from Table 1, the energy required for ignition of H 2 is 1/10 of that of CH 4 , and if a catalyst is used, it can be ignited even at room temperature. It is the fastest and requires the least amount of air for combustion. On the other hand, CH 4 has a high ignition temperature, a slow combustion speed, and the amount of air required for combustion is three times that of H 2 . The present inventors used the above two types of fuel, and the fifth
Various experiments were carried out using the catalytic burner type reformer shown in the figure, and the following results were clarified. (1) When the amount of air was constant and only the amount of H 2 was increased (H 2 concentration relative to air from 1.2 to 1.5%), the temperature only in the catalytic burner section increased (see Figure 6). In the diagram, C
indicates the case where the amount of H2 is small, and D indicates the case where the amount of H2 is large. (2) When only the amount of CH 4 was increased (CH 4 concentration relative to air from 1.5% to 2.3%) while the amount of air remained constant, the temperature in the catalytic burner part did not rise much, and the highest temperature part moved to the heat transfer particle layer ( (See Figure 7). In the figure, E
indicates the case where the amount of CH 4 is small, and F indicates the case where the amount of CH 4 is maximum. (3) When the flow velocity of the combustion section was increased by adjusting the amount of combustion air (from about 0.2 m/s to 0.3 m/s superficial velocity of the combustion section), the maximum temperature range increased as the flow velocity increased. The trend was shown (see Figure 8). In the figure, G indicates a case where the flow velocity (air amount) is low, and H indicates a case where the flow velocity is high. In addition, the reaction part is an endothermic reaction, but when we investigated the distribution of the amount of heat absorbed, we found that the reaction part temperature was 650.
It was found that the largest amount of heat absorption was observed at a temperature of ~700°C, resulting in a large heat flux. Based on the above results, it was conventionally thought that hot spots occur when fuel is directly supplied to the catalyst layer, but this is caused by the combustion of H 2 with a high burning rate, and it takes time for CH 4 to be completely burned. It was found that the mixture spreads into the packed bed and then combusts. In addition, the combustion gas in a conventional re-former is flowed in a countercurrent flow to the gas in the reaction section, but the outlet temperature of the reaction section is
Since the temperature is 750-800℃, there is a sensible heat rise from the 650-700℃ range forming a significant endothermic zone to the outlet temperature, and the sensible heat of the combustion gas is used for this sensible heat increase. ), the temperature of the combustion gas decreases, making it impossible to maintain a large enough temperature difference between the zone and the reaction zone, and it was therefore found that the heat transfer surface must be increased. The re-former shown in FIG. 5 is provided with a supply pipe 15A for high-calorie fuel gas (for example, natural gas, CH 4 ) in the combustion part (filling part) corresponding to the heat absorption part (reaction part) of the reaction tube, and also in the combustion part. From the bottom, the packed beds are: combustion catalyst first layer 18A, heat transfer particle layer first layer 19
A, heat transfer particle layer second layer 19B, combustion catalyst second layer 1
8B, a third heat transfer particle layer 19C and a metal particle layer 19M, anode waste gas (hydrogen gas) is supplied from the low calorie fuel gas supply pipe 15 at the bottom of the reactor, and from the high calorie fuel supply pipe 15A at the top. No. 13 in that it started supplying natural gas (CH 4 ).
This is different from the conventional device shown in the figure. In an apparatus with such a configuration, H 2 having a high combustion rate is introduced from the gas supply pipe 15 into the fuel/air premixing zone 17, where it is mixed with the air supplied from the air supply pipe 16, and the combustion catalyst first It enters the layer (catalytic burner) 18A and is burned here,
The combustion heat is used for heat transfer to the tip of the reaction tube 14. Heat transfer at the tip of the reaction tube 14 is mainly used to increase the sensible heat of the reaction fluid past the heat absorption zone. The combustion gas in the combustion catalyst first layer 18A gives heat to the reaction section of the reaction tube in the heat transfer particle layer first layer 19A, and its temperature is lowered. The combustion gas whose temperature has been lowered then enters the endothermic zone and is heated by the combustion heat of the high-calorie fuel supplied from the fuel supply pipe 15A at the center of the reaction tube. That is, the fuel supply pipe 15 is used to heat the reaction section (endothermic zone) of the reaction tube.
CH 4 supplied from A and having a slow burning rate is used. The part to which this CH 4 is supplied has a packed bed of heat transfer particles with no combustion activity (heat transfer particle layer 2 layer 19).
Since B) is filled, it is sufficiently diffused into the filled part before being completely combusted in the combustion catalyst part on the upstream side. The filling material of this second heat transfer particle layer 19B is
It is preferable to make the diameter larger so that CH 4 can easily diffuse. The CH 4 thus diffused into the filling part enters the combustion catalyst second layer 18B on the downstream side thereof and is combusted all at once. The position of the second layer of combustion catalyst is set so that the temperature of the reaction section is around 650°C during normal operation. A third heat transfer particle layer is further provided on the second combustion catalyst layer 18B, and a metal particle layer 19M is further provided thereon.
The position where the metal particle layer 19M is switched is preferably such that the combustion gas temperature decreases to about 700°C. The metal particles of the metal particle layer 19M have lower heat resistance than the heat transfer particle layer 19C made of a refractory material such as alumina, and also lead to an increase in weight, but as shown in FIG. 9, the metal particles have a high thermal conductivity. , the heat transfer coefficient can be improved. Furthermore, since metal particles have a high density, they also have the effect of preventing light refractory particles from scattering when the flow rate increases. Note that the heat transfer coefficient of the packed bed exhibits a larger value as the particle size becomes larger in a high temperature region where radiation is large.
Therefore, the heat transfer particle layers 19A and 19 at the bottom of the reactor
It is preferable that the particles of B have a larger diameter than the particles of the upper heat transfer particle layer 19C. Next, temperature control of the reaction section and combustion section of the catalytic combustion reactor will be explained using FIG. 10 and FIG. 11. A plurality of thermocouples are used to measure the temperature inside the reaction column at equal intervals in the axial direction of the reaction tube (in this case, thermocouples A, B,
Thermocouples A', B', C', D' and E' are attached to the surrounding combustion section (filling section) at the same height as the reaction section. Furthermore, a thermocouple F for protecting the reaction tube is attached to the surface of the reaction tube in the reaction tube return section. Each dimension is determined at the time of design so that the heat absorption zone of the reaction section is located between the thermocouples C and D, and the fuel supply pipe 15A is arranged so as to be approximately at the same height as the thermocouple D. The air supply pipe 16 has an air flow control valve 47.
However, the upper and lower fuel supply pipes 15A and 1
5 each has a natural gas (CH 4 ) flow rate control valve 48.
and a lower natural gas flow rate control valve 49 are provided, respectively, and these are respectively connected to the electric circuits of the thermocouples that are electrically connected to the air flow rate control valve 47. In such a configuration, the fuel and air control method is as follows. First, read the indicated values of thermocouples A to E and write the temperature profile of the reaction section in the computer. Next, read the readings from the thermocouples A' to D' and write the temperature profile of the combustion section into the computer. Next, overlap the temperature profiles of both sides,
The CH 4 valves 48 and 49 and the air valve 47 are adjusted so that the endothermic zone of the reaction section and the maximum combustion temperature due to CH 4 combustion overlap. The amount of air at this time is
The theoretical combustion temperature of 18B and 18B does not exceed the heat-resistant limit temperature of the catalyst, and the amount to suppress the excess air ratio as much as possible is calculated in advance, and an appropriate amount of air is supplied through the valve 47 according to the amount of CH 4 supplied. supply
Valves 48 and 49 are used to raise and lower the maximum temperature of the combustion section. That is, when raising the maximum part, valve 49 is closed and valve 48 is opened, while when lowering the maximum part, valve 49 is closed and valve 48 is opened.
9 and close valve 48. Further, during load fluctuation operation, the heat absorption zone may be separated from between thermocouples C and D, but the combustion section is similarly controlled by opening and closing valves 48 and 49. By controlling the temperature of such two-stage combustion, a large amount of heat can be effectively provided to the endothermic zone where heat is required, and the heat transfer area can be minimized. FIG. 12 shows an example of a specific control program for the computer. Among these, the endothermic zone is determined by using the indicated values of thermocouples A to E.
The values on both sides of 650℃ and 700℃ are detected, and the space between them is defined as the endothermic zone. For example, C is 620℃,
When D is 710°C, zone 3 sandwiched between CD is an endothermic zone. Also, the temperature maximum value Tp of the combustion zone
To find out, determine the maximum temperature value from A' to D' excluding E', and set it as the maximum temperature value Tp. For example, if C' is the maximum value, C' becomes Tp. Next, to determine whether Tp is below the endothermic zone, in this case, C′ is Tp
Therefore, Tp is above the endothermic zone. The operation is to squeeze the valve 48 and open the valve 49. As a result, the catalytic burner (first stage combustion catalyst) side is heated, and Tp decreases. Tube temperature F
The set value of is determined based on the design temperature of the reaction tube. This program is run at appropriate intervals (for example, 1 minute)
Let it be an infinite loop that repeats with . For example, if Tp drops to D' at the next time, then valve 4
8 is opened, valve 49 is squeezed, and Tp rises. In other words, Tp slowly moves back and forth between the upper and lower ends of the endothermic zone. According to the above embodiment, by effectively heating the endothermic zone of the reaction section, the heat transfer area can be made smaller by, for example, 20 to 40% than in conventional re-formers, and the amount of combustion air can be suppressed. Therefore, the sensible heat taken out of the exhaust gas decreases, and the thermal efficiency improves, for example.
Improve by 10-20%. Furthermore, high efficiency operation is possible under any load condition by controlling the temperature profiles of the reaction section and combustion section. (Effects of the Invention) According to the present invention, in a catalyst-filled reformer, fuel gas is supplied from at least two locations, one at the bottom of the packed bed of the reactor and the other at the top thereof, and the diameter of the packed particles in the fuel supply section is increased. This makes it possible to improve heat transfer performance and make the temperature of the reaction tube in the reforming reaction zone uniform. In addition, for example, low-calorie and high-calorie fuels can be supplied from the two fuel supply sections mentioned above, and the catalyst filling By alternately providing the combustion catalyst layer and the heat transfer particle layer, the reforming reaction zone, that is, the endothermic zone, can be effectively heated, the heat transfer area can be reduced, and the amount of combustion air can be reduced. It is possible to reduce sensible heat taken out of exhaust gas and improve thermal efficiency.

【図面の簡単な説明】[Brief explanation of the drawing]

第1図は、本発明の一実施例を示す改質反応器
の説明図、第1−A図および第1−B図は、それ
ぞれ第1図のA−A′線に沿う矢視方向の断面図、
第2図は、第1図の装置における反応管高さに対
する反応管の表面温度を示す図、第3図および第
4図は、それぞれ伝熱係数に及ぼす温度および粒
径の関係を示す図、第5図は、本発明の他の実施
例を示す改質反応器の断面図、第6図、第7図お
よび第8図は、それぞれ上記改質反応器の燃料と
してH2、CH4、並びに空気量の変化に対する燃
焼部の温度プロフイルの変化を示す図、第9図
は、改質反応器の伝熱粒子の熱伝導率と充填層の
総括伝熱係数の関係を示す図、第10図は、本発
明の燃料分割供給方式の改質反応器の温度制御の
系統を示す図、第11図は、第10図の温度制御
における制御パターンを示す説明図、第12図
は、同じく上記温度制御の制御プログラムのフロ
ーチヤートを示す図、第13図は、従来の改質反
応器の典型例を示す説明図、第14図は、燃料電
池のアノード廃ガスおよびカソード廃空気を利用
した改質反応器の装置系統図である。 31……改質反応器、32……燃料ガス供給
口、33……空気供給口、34……反応管、35
……燃焼廃ガス排出口、36……原料ガス供給
口、37……生成ガス排出口、38……触媒粒
子、39……低温ゾーン、40……高温ゾーン、
41……塔中央部燃料ガス供給口、42……大粒
径触媒、43……反応管内管、47……空気流量
調節弁、48,49……天然ガス流量調節弁、1
1……原料供給管、12……改質触媒層、13…
…反応管(外管)、14……反応管(内管)、15
……燃料ガス供給管、16……空気供給管、17
……燃料、空気予混合ゾーン、18A……燃焼触
媒第1層、19A……伝熱粒子層第1層、20…
…燃焼廃ガス排出口、15A……CH4供給管、1
8B……燃焼触媒第2層、21……改質ガス出
口、19B……伝熱粒子層第2層、19C……伝
熱粒子第3層、19M……金属粒子層。
FIG. 1 is an explanatory diagram of a reforming reactor showing one embodiment of the present invention, and FIGS. 1-A and 1-B are respectively taken in the direction of the arrow along line A-A' in FIG. cross section,
FIG. 2 is a diagram showing the surface temperature of the reaction tube with respect to the reaction tube height in the apparatus of FIG. 1, and FIGS. 3 and 4 are diagrams showing the relationship between temperature and particle size on the heat transfer coefficient, respectively. FIG. 5 is a sectional view of a reforming reactor showing another embodiment of the present invention, and FIGS. 6, 7, and 8 show H 2 , CH 4 , FIG. 9 shows the relationship between the thermal conductivity of heat transfer particles in the reforming reactor and the overall heat transfer coefficient of the packed bed. 11 is an explanatory diagram showing the control pattern in the temperature control of FIG. 10, and FIG. 12 is a diagram showing the temperature control system of the reforming reactor of the fuel split supply system of the present invention. FIG. 13 is an explanatory diagram showing a typical example of a conventional reforming reactor, and FIG. 14 is a flowchart of a control program for temperature control. FIG. 2 is an apparatus system diagram of a quality reactor. 31... Reforming reactor, 32... Fuel gas supply port, 33... Air supply port, 34... Reaction tube, 35
... Combustion waste gas discharge port, 36 ... Raw material gas supply port, 37 ... Produced gas discharge port, 38 ... Catalyst particles, 39 ... Low temperature zone, 40 ... High temperature zone,
41... Tower central fuel gas supply port, 42... Large particle size catalyst, 43... Reaction tube inner tube, 47... Air flow rate control valve, 48, 49... Natural gas flow rate control valve, 1
1... Raw material supply pipe, 12... Reforming catalyst layer, 13...
...Reaction tube (outer tube), 14...Reaction tube (inner tube), 15
... Fuel gas supply pipe, 16 ... Air supply pipe, 17
... Fuel, air premixing zone, 18A ... Combustion catalyst first layer, 19A ... Heat transfer particle layer first layer, 20 ...
...Combustion waste gas outlet, 15A...CH 4 supply pipe, 1
8B...Combustion catalyst second layer, 21...Reformed gas outlet, 19B...Second heat transfer particle layer, 19C...Third heat transfer particle layer, 19M...Metal particle layer.

Claims (1)

【特許請求の範囲】 1 触媒および伝熱粒子を充填した反応器に反応
管を挿入し、該触媒および伝熱粒子の充填部に燃
料ガスを供給して燃焼させ、前記反応管を加熱し
て該管内を通る原料を分解、改質する装置におい
て、前記反応管の下部と反応部の位置の触媒およ
び伝熱粒子充填部の少なくとも2個所に燃料ガス
を供給する手段を設け、少なくとも前記反応部に
相当する充填部の粒子径を他の部分のそれよりも
大にしたことを特徴とする触媒燃焼式反応器。 2 特許請求の範囲第1項において、前記充填部
を燃焼触媒と伝熱粒子の層状構造とし、少なくと
も前記反応部に相当する触媒充填部の触媒粒子径
を他の部分のそれよりも大としたことを特徴とす
る触媒燃焼式反応器。 3 触媒および伝熱粒子を層状に充填した反応器
に反応管を挿入し、該反応管の下部と反応部の位
置の触媒充填層の少なくとも2個所に燃料ガスを
供給して燃焼させ、前記反応管を加熱して該管内
を通る原料を分解、改質する触媒燃焼式反応器の
燃焼方法において、前記反応管の反応部に相当す
る触媒充填層に供給する燃料ガスを一旦触媒充填
層の下層の伝熱粒子層に供給し、該燃焼ガスを充
填層全体に広げた後、前記触媒充填層に流入させ
ることを特徴とする触媒燃焼式反応器の燃焼方
法。 4 特許請求の範囲第3項において、前記反応管
の反応部の位置の触媒充填層に供給される燃焼ガ
スの供給量に対して一定の関係で燃焼ガス速度が
得られるように該触媒充填層の空気量を調節する
ことを特徴とする触媒燃焼式反応器の燃焼方法。 5 特許請求の範囲第3項において、前記反応部
と該反応部の位置の充填部に温度センサーを設
け、該反応部の温度が650〜700℃になる位置にお
いて充填部の温度が極大値をとるように該充填部
の燃料供給量を調整することを特徴とする触媒燃
焼式反応器の燃焼方法。
[Claims] 1. A reaction tube is inserted into a reactor filled with a catalyst and heat transfer particles, and fuel gas is supplied to the portion filled with the catalyst and heat transfer particles to cause combustion, thereby heating the reaction tube. In the apparatus for decomposing and reforming the raw material passing through the tube, means is provided for supplying fuel gas to at least two locations: a lower part of the reaction tube and a catalyst and heat transfer particle filling section located at the reaction section; 1. A catalytic combustion reactor characterized in that the particle size of the packed part corresponding to 2 is larger than that of other parts. 2. In claim 1, the packed section has a layered structure of a combustion catalyst and heat transfer particles, and the catalyst particle diameter of at least the catalyst packed section corresponding to the reaction section is larger than that of other parts. A catalytic combustion reactor characterized by: 3. A reaction tube is inserted into a reactor filled with a catalyst and heat transfer particles in a layered manner, and fuel gas is supplied to at least two places, the lower part of the reaction tube and the catalyst packed bed at the reaction part, to be combusted, and the reaction is started. In a combustion method for a catalytic combustion reactor in which a tube is heated to decompose and reform the raw material passing through the tube, the fuel gas supplied to the catalyst packed bed corresponding to the reaction section of the reaction tube is temporarily transferred to the lower layer of the catalyst packed bed. A combustion method for a catalytic combustion reactor, characterized in that the combustion gas is supplied to a heat transfer particle bed, and after spreading the combustion gas throughout the packed bed, it flows into the catalyst packed bed. 4. In claim 3, the catalyst packed bed is arranged such that the combustion gas velocity is maintained in a constant relationship with the amount of combustion gas supplied to the catalyst packed bed at the reaction section of the reaction tube. A combustion method for a catalytic combustion reactor characterized by adjusting the amount of air. 5 In claim 3, a temperature sensor is provided in the reaction part and a filling part at the position of the reaction part, and the temperature of the filling part reaches a maximum value at a position where the temperature of the reaction part becomes 650 to 700°C. A combustion method for a catalytic combustion reactor, characterized in that the amount of fuel supplied to the filling section is adjusted so as to increase the amount of fuel supplied to the filling section.
JP22859484A 1984-10-30 1984-10-30 Catalytic combustion type reactor and its operation Granted JPS61106402A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP22859484A JPS61106402A (en) 1984-10-30 1984-10-30 Catalytic combustion type reactor and its operation

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP22859484A JPS61106402A (en) 1984-10-30 1984-10-30 Catalytic combustion type reactor and its operation

Publications (2)

Publication Number Publication Date
JPS61106402A JPS61106402A (en) 1986-05-24
JPH059362B2 true JPH059362B2 (en) 1993-02-04

Family

ID=16878799

Family Applications (1)

Application Number Title Priority Date Filing Date
JP22859484A Granted JPS61106402A (en) 1984-10-30 1984-10-30 Catalytic combustion type reactor and its operation

Country Status (1)

Country Link
JP (1) JPS61106402A (en)

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19855769B4 (en) * 1998-12-03 2008-10-09 Nucellsys Gmbh Catalytically heated component for a chemical reactor
JP5154993B2 (en) * 2007-09-13 2013-02-27 Jx日鉱日石エネルギー株式会社 Reformer

Also Published As

Publication number Publication date
JPS61106402A (en) 1986-05-24

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