JP2008069029A - Method for staring-up reformer - Google Patents
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- JP2008069029A JP2008069029A JP2006247943A JP2006247943A JP2008069029A JP 2008069029 A JP2008069029 A JP 2008069029A JP 2006247943 A JP2006247943 A JP 2006247943A JP 2006247943 A JP2006247943 A JP 2006247943A JP 2008069029 A JP2008069029 A JP 2008069029A
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- 238000000034 method Methods 0.000 title claims abstract description 31
- 238000002485 combustion reaction Methods 0.000 claims abstract description 93
- 239000007789 gas Substances 0.000 claims abstract description 45
- 238000002407 reforming Methods 0.000 claims abstract description 33
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 19
- 239000000446 fuel Substances 0.000 claims description 19
- 229910052739 hydrogen Inorganic materials 0.000 claims description 7
- 239000001257 hydrogen Substances 0.000 claims description 7
- 238000009529 body temperature measurement Methods 0.000 claims description 3
- 125000004435 hydrogen atom Chemical class [H]* 0.000 claims 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 6
- 239000000126 substance Substances 0.000 abstract description 3
- 239000003054 catalyst Substances 0.000 description 17
- 238000006243 chemical reaction Methods 0.000 description 8
- 239000000567 combustion gas Substances 0.000 description 7
- 239000004215 Carbon black (E152) Substances 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 4
- 229910002091 carbon monoxide Inorganic materials 0.000 description 4
- 229930195733 hydrocarbon Natural products 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 230000004913 activation Effects 0.000 description 3
- 238000010586 diagram Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 239000002737 fuel gas Substances 0.000 description 2
- 238000012886 linear function Methods 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000007084 catalytic combustion reaction Methods 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- -1 city gas Chemical class 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000003350 kerosene Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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- Fuel Cell (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
Description
本発明は、都市ガス、LPガス、灯油等の炭化水素化合物を、燃焼部を有する改質器にて改質して水素を生成する改質器の起動方法に関する。 The present invention relates to a method for starting a reformer that generates hydrogen by reforming a hydrocarbon compound such as city gas, LP gas, or kerosene in a reformer having a combustion section.
炭化水素化合物を改質して水素を生成する改質器は、水素化社会の形成に向けて重要な装置であり、近年、種々の分野で多く採用され始めている。特に、改質水素を燃料ガスとする燃料電池発電装置においては不可欠である。即ち、燃料電池本体に供給される燃料ガスとして、燃料改質器にて天然ガス等の炭化水素系あるいはメタノール等のアルコール系の原燃料を改質触媒の下で水素に富むガスに改質した改質ガスが使用される。 A reformer that reforms a hydrocarbon compound to produce hydrogen is an important device for the formation of a hydrogenated society, and has recently begun to be widely adopted in various fields. In particular, it is indispensable in a fuel cell power generation apparatus using reformed hydrogen as fuel gas. That is, as a fuel gas supplied to the fuel cell main body, a hydrocarbon-based raw fuel such as natural gas or an alcohol-based raw fuel such as methanol is reformed into a gas rich in hydrogen under a reforming catalyst in a fuel reformer. A reformed gas is used.
炭化水素化合物を改質するには改質触媒を改質可能な温度にまで昇温しなければならない。そこで改質器中に燃焼部を設け、燃焼部で炭化水素化合物と空気を混合して燃やすことにより発生した燃焼熱を改質触媒層に伝熱することにより昇温する改質器の起動方法が一般的に行なわれている。 In order to reform the hydrocarbon compound, it is necessary to raise the temperature of the reforming catalyst to a temperature capable of reforming. Therefore, a reformer start-up method for raising the temperature by providing a combustion section in the reformer and transferring the combustion heat generated by mixing and burning the hydrocarbon compound and air to the reforming catalyst layer in the combustion section. Is generally done.
特許文献1には、「内管とこれを囲む外管との間に触媒層を内蔵する円筒式の反応管をバーナによる燃焼で生じた熱媒体により加熱して炭化水素系の原燃料を改質する燃料改質器の起動停止のヒートサイクルの際、起動時に生じる内管と外管との熱膨脹差による触媒層にかかる圧縮力を小さくして触媒の圧壊を減少すること」を目的として、「燃料改質器の起動時、バーナによる燃焼量を燃焼開始から順次増加する、この方法として燃焼量を階段状に順次増加させ、内管と外管との温度差を小さくする改質器の起動方法」が開示されている。 Patent Document 1 states that “a cylindrical reaction tube containing a catalyst layer between an inner tube and an outer tube surrounding the inner tube is heated by a heat medium generated by combustion by a burner to modify a hydrocarbon-based raw fuel. For the purpose of reducing the compression of the catalyst by reducing the compressive force applied to the catalyst layer due to the difference in thermal expansion between the inner tube and the outer tube that occurs during startup during the heat cycle of starting and stopping the fuel reformer “When the fuel reformer starts up, the amount of combustion by the burner is gradually increased from the start of combustion. As a method of this, the amount of combustion is increased stepwise and the temperature difference between the inner and outer tubes is reduced. An “activation method” is disclosed.
特許文献1に開示された改質器の構成とその起動方法について、特許文献1の記載を一部引用して、以下にその概要を述べる。図3は、特許文献1において図7として開示された円筒式の反応管を備えた燃料改質器の断面図である。なお、図3に示す改質器は、本発明の対象とする改質器の一例でもある。図3において炉容器10は上部中央にバーナタイル11に囲まれたバーナ12と、側壁上部にバーナ12からの燃料が燃焼して生じる燃焼ガスを排出する排ガス出口13とを備え、さらに反応管21を有する改質管14を内蔵している。
About the structure of the reformer disclosed in Patent Document 1 and the starting method thereof, the description of Patent Document 1 will be partially cited and the outline thereof will be described below. FIG. 3 is a cross-sectional view of a fuel reformer provided with a cylindrical reaction tube disclosed in FIG. Note that the reformer shown in FIG. 3 is also an example of a reformer targeted by the present invention. In FIG. 3, a
改質管14はバーナ12がその内側に臨む内管15と、これを囲む外囲管16と、この下部開口部を閉鎖する底板17と、内管15と外囲管16との間に底板17から離して介挿される外管18とから構成され、内管15と外管18との間の環状空間には改質触媒19が充填されてなる触媒層20を内蔵して反応管21が形成されている。なお、外管18と外囲管16との間は改質原料ガスが流れる改質原料ガス通路22を形成している。
The reforming
改質管14の外管18と外囲管16との上部開口は炉容器10の上部に設けられた改質原料ガスマニホールド23に連通し、改質原料ガスマニホールド23は改質原料ガスが流入する改質原料ガス入口24を備えている。また内管15と外管18との上部開口は炉容器10の上部に設けられた改質ガスマニホールド25に連通し、改質ガスマニホールド25は改質ガスを外部に送出する改質ガス出口26を備えている。なお、内管15の内側は燃焼室27を形成し、外囲管16と炉容器10との間は燃焼ガス通路28を形成している。
The upper openings of the outer tube 18 and the outer tube 16 of the reforming
このような構成により、バーナ12からの燃料を燃焼させると燃焼ガスは矢印のように内管15の内側面に沿って燃焼室27を下方に流れ、改質管14の下端部で折返して外囲管16の外側面に沿って燃焼ガス通路28を流れて反応管21を有する改質管24を加熱した後、排ガス出口13から外部に排出される。
With such a configuration, when the fuel from the
一方、改質原料ガスは、改質原料ガス入口24から改質原料ガスマニホールド23を経て改質原料ガス通路22を下方に流れ、その下端部で触媒層20に流入する。そして改質原料ガスは燃焼ガスにより加熱された触媒層20を下方から上方に向かって流れ、触媒作用の下に水素に富むガスに水蒸気改質されて改質ガスマニホールド25を経て改質ガス出口26から燃料電池に送出される。
On the other hand, the reforming source gas flows downward from the reforming
なお、上記のような燃料改質器を冷状態から起動するときにはつぎのようにして行われる。燃焼開始時は燃焼量を従来の燃焼量より少なくし、起動時間の経過に伴って燃焼量をA,B,C,Dのように階段状にして増加する。図2は、特許文献1において図1として開示された改質器の起動方法に係り、燃焼量と起動時間との関係を概念的に示す図である。 In addition, when starting the above fuel reformer from a cold state, it is performed as follows. At the start of combustion, the combustion amount is made smaller than the conventional combustion amount, and the combustion amount is increased stepwise like A, B, C, D as the start-up time elapses. FIG. 2 is a diagram conceptually showing the relationship between the combustion amount and the startup time in the reformer startup method disclosed in FIG.
ところで、上記特許文献1の発明のように、経過時間に従い燃焼量を階段状に増加する場合、下記のような問題がある。
(1)外気温が高温の場合と低温の場合では改質器の昇温にかかる時間が変化してしまう。(2)改質器を構成する燃焼ガス通路や燃焼排ガス配管が十分に昇温する前に燃焼量を増加すると安定に燃焼せず不完全燃焼を引起し、燃えずに排出した炭化水素化合物を含む可燃性ガスや一酸化炭素が基準値以上排出される問題がある。安定に燃焼しない原因としては改質器を構成する燃焼ガス通路や燃焼排ガス配管が十分に昇温する前に高温の排ガスを流通させると排ガスが冷やされ凝縮することで圧力振動や流量変動を引起し燃焼部で失火を引起す。失火後も燃焼部の着火装置が継続して動作していると着火と失火を繰返し、安定燃焼しない。
(3)安定燃焼しないと燃焼熱の発生も少なく改質器の昇温にも時間がかかる。また投入した炭化水素化合物を燃やしきらないため起動エネルギーも過剰に必要である。
(1) When the outside air temperature is high and when it is low, the time required for raising the temperature of the reformer changes. (2) If the combustion amount is increased before the temperature of the combustion gas passage and combustion exhaust gas pipe constituting the reformer is sufficiently increased, the combustion does not occur stably, causing incomplete combustion, and the hydrocarbon compounds discharged without burning There is a problem that combustible gas and carbon monoxide contained are discharged more than the standard value. The reason why combustion does not occur stably is that if high-temperature exhaust gas is circulated before the temperature of the combustion gas passage and combustion exhaust gas pipe constituting the reformer is sufficiently raised, the exhaust gas is cooled and condensed, causing pressure fluctuations and flow fluctuations. Causes misfire in the burner. If the ignition device in the combustion section continues to operate even after a misfire, ignition and misfire are repeated, and stable combustion does not occur.
(3) If stable combustion is not performed, combustion heat is hardly generated and it takes time to raise the temperature of the reformer. In addition, excessive activation energy is required because the injected hydrocarbon compound cannot be burned.
本発明は、上記の問題点に鑑みてなされたもので、この発明の課題は、起動時間を短縮し、改質器を昇温する過程で燃焼部から排気される燃焼排ガス中に含まれる有害物質を低減するとともに、改質器の起動に要するエネルギー量を低減することが可能な改質器の起動方法を提供することにある。 The present invention has been made in view of the above-described problems, and an object of the present invention is to reduce the start-up time and to prevent harmful emissions contained in the combustion exhaust gas exhausted from the combustion section in the process of raising the temperature of the reformer. An object of the present invention is to provide a method for starting a reformer capable of reducing substances and reducing the amount of energy required for starting the reformer.
上記課題は、以下により達成される。即ち、炭化水素化合物を、燃焼部を有する改質器にて改質して水素を生成する改質器の起動方法であって、炭化水素化合物と燃焼用空気とを前記燃焼部で燃焼することによって発生する燃焼熱により改質器の温度を上昇させ、前記燃焼部における燃焼量を燃焼開始から起動時間経過に伴って順次増加させ改質器の温度を改質に適する所定の温度に昇温する改質器の起動方法において、改質器の起動時において、前記燃焼量を、改質器の予め定めた所定位置における温度測定値に基づいて制御することをことを特徴とする(請求項1)。 The above-mentioned subject is achieved by the following. That is, a reformer start-up method in which a hydrocarbon compound is reformed by a reformer having a combustion section to generate hydrogen, and the hydrocarbon compound and combustion air are combusted in the combustion section. The temperature of the reformer is raised by the combustion heat generated by the fuel, and the amount of combustion in the combustion section is gradually increased with the start-up time from the start of combustion, and the temperature of the reformer is raised to a predetermined temperature suitable for reforming. In the reformer starting method, the combustion amount is controlled based on a temperature measurement value at a predetermined position of the reformer when the reformer is started. 1).
また、前記請求項1の発明の実施態様としては、下記請求項2ないし4の発明が好ましい。即ち、前記請求項1に記載の起動方法において、起動初期においては、所定の炭化水素化合物および燃焼用空気量に基づく所定の燃焼量により、燃焼量を変化させずに改質器の温度を上昇させ、前記温度測定値が所定の温度に到達した際には、燃焼量を時間の経過とともに比例的に増加させ、その後、改質器の温度を改質に適する所定の温度に昇温する(請求項2)。 As an embodiment of the invention of claim 1, the inventions of claims 2 to 4 are preferable. That is, in the start-up method according to claim 1, at the initial stage of start-up, the temperature of the reformer is increased without changing the combustion amount by a predetermined combustion amount based on the predetermined hydrocarbon compound and the amount of combustion air. When the measured temperature value reaches a predetermined temperature, the combustion amount is increased proportionally with the passage of time, and then the temperature of the reformer is raised to a predetermined temperature suitable for reforming ( Claim 2).
さらに、前記請求項1または2に記載の起動方法において、前記温度測定を行なう所定位置は、改質器の燃焼部から大気に燃焼排ガスを排出する配管部とする(請求項3)。また、前記請求項1ないし3のいずれか1項に記載の起動方法において、前記改質器は、燃料電池発電装置に使用されるものとする(請求項4)。 Furthermore, in the start-up method according to claim 1 or 2, the predetermined position where the temperature is measured is a pipe part for discharging combustion exhaust gas from the combustion part of the reformer to the atmosphere (claim 3). In the start-up method according to any one of claims 1 to 3, the reformer is used in a fuel cell power generator (claim 4).
なお、本発明において、改質器の構成は、前記図3に記載された構成には限定されない。改質器の構成としては、一般に、反応管の形式(単管式、二重管式、円筒式等)、燃焼部の形式(バーナ、触媒燃焼、配置が上部か下部か等)など、全体構成にわたって種々相違するものが知られているが、本発明においては特定の改質器構成に限定されるものではない。また、測定する改質器の温度としては、上記配管部の温度には限定されない。改質触媒の温度や反応管の温度など、改質器を代表する場所の温度であれば適宜採用できる。 In the present invention, the configuration of the reformer is not limited to the configuration described in FIG. In general, the reformer configuration includes the type of reaction tube (single tube type, double tube type, cylindrical type, etc.), the type of combustion part (burner, catalytic combustion, whether the arrangement is upper or lower), etc. Although various differences are known over the configuration, the invention is not limited to a specific reformer configuration. Further, the temperature of the reformer to be measured is not limited to the temperature of the pipe section. Any temperature that represents the reformer, such as the temperature of the reforming catalyst or the temperature of the reaction tube, can be used as appropriate.
この発明によれば、改質器の起動時に燃焼部に導入する炭化水素化合物と燃焼用空気の燃焼量をまず安定に燃焼できる量から燃焼を開始し、次に改質器の温度、例えば改質触媒の温度や排ガス配管の温度測定値に基づいて燃焼量を増加することにより、燃焼部の失火を防ぎ、安定燃焼させることで可燃性ガスや一酸化炭素の排出量を基準値以下に抑え、起動時間を短縮し、かつ起動エネルギーも低減できる。 According to the present invention, combustion starts from a quantity capable of stably combusting the hydrocarbon compound and combustion air introduced into the combustion section when the reformer is started, and then the reformer temperature, for example, the reformer By increasing the amount of combustion based on the temperature of the catalyst and the temperature of the exhaust gas pipe, the misfire of the combustor is prevented, and the amount of combustible gas and carbon monoxide is reduced below the reference value by stable combustion. , Start-up time can be shortened and start-up energy can be reduced.
次に、この発明の実施形態に関して、図1に基いて説明する。図1は本発明の実施形態に係る改質器の起動方法における燃焼量の増加方法を模式的に示す図である。以下に、起動方法の実施例を示す。下記の実施例における改質器の構成は前記図3に示すものと同等である。いずれの実施例においても、図1に示すような燃焼量の増加方法とすることにより、所期の改質器の起動方法が実現できることが確認された。 Next, an embodiment of the present invention will be described with reference to FIG. FIG. 1 is a diagram schematically showing a combustion amount increasing method in a reformer start-up method according to an embodiment of the present invention. An example of the activation method is shown below. The structure of the reformer in the following embodiment is the same as that shown in FIG. In any of the examples, it was confirmed that the intended reformer start-up method can be realized by using the combustion amount increasing method as shown in FIG.
着火時には安定燃焼させるため、炭化水素系燃料(都市ガス)を0.3 NL/minの流量、燃焼用空気を5.6 NL/minの流量で、改質器の燃焼部に導入しイグナイタにより着火した。そして図3に示す改質触媒19の温度(触媒層における改質ガス出口部の触媒温度)が150℃になるまで燃焼量を変化させずに昇温した。その後、改質触媒19の温度が150℃から540℃の間は都市ガスを0.3〜0.8 NL/minへ、燃焼用空気は5.6〜16 NL/minへと一次関数的に増加させ、改質器の昇温を行った。
In order to ensure stable combustion during ignition, hydrocarbon fuel (city gas) was introduced into the combustion section of the reformer at a flow rate of 0.3 NL / min and combustion air at a flow rate of 5.6 NL / min and ignited by an igniter. The temperature was raised without changing the amount of combustion until the temperature of the reforming
着火時には安定燃焼させるため、炭化水素系燃料(都市ガス)を0.3 NL/minの流量、燃焼用空気を5.6 NL/min改質器の燃焼部に導入しイグナイタにより着火した。そして図3に示す改質器燃焼部の排気ガス配管13の温度が40℃になるまで燃焼量を変化させずに昇温した。排気ガス配管13の温度が40℃から60℃の間は都市ガスを0.3〜0.8 NL/minへ、燃焼用空気は5.6〜16 NL/minへと一次関数的に増加させ、改質器の昇温を行った。
In order to ensure stable combustion during ignition, hydrocarbon fuel (city gas) was introduced at a flow rate of 0.3 NL / min and combustion air was introduced into the combustion section of the 5.6 NL / min reformer and ignited by an igniter. Then, the temperature was raised without changing the combustion amount until the temperature of the
表1は、上記本発明の実施例のように燃焼部が安定燃焼している時と、従来技術におけるように着火と失火を繰り返している時の排ガス中に含まれる一酸化炭素(CO)濃度と、燃焼せずに排出された排ガス中可燃性ガス濃度を示す。いずれの濃度も、本発明の場合の方が、従来技術に比較して格段に小さい値を示す。 Table 1 shows the concentration of carbon monoxide (CO) contained in the exhaust gas when the combustion section is stably combusting as in the embodiment of the present invention and when ignition and misfire are repeated as in the prior art. And the concentration of combustible gas in the exhaust gas discharged without combustion. All the concentrations are much smaller in the case of the present invention than in the prior art.
12:バーナ、13:燃焼排ガス出口、19:改質触媒、21:反応管。 12: Burner, 13: Combustion exhaust gas outlet, 19: Reforming catalyst, 21: Reaction tube.
Claims (4)
改質器の起動時において、前記燃焼量を、改質器の予め定めた所定位置における温度測定値に基づいて制御することを特徴とする改質器の起動方法。 A reformer start-up method in which a hydrocarbon compound is reformed by a reformer having a combustion section to generate hydrogen, and is generated by burning the hydrocarbon compound and combustion air in the combustion section. The temperature of the reformer is increased by the combustion heat generated, and the amount of combustion in the combustion section is sequentially increased as the start-up time elapses from the start of combustion, and the temperature of the reformer is increased to a predetermined temperature suitable for reforming. In the starting method of the instrument,
A method for starting a reformer, characterized in that, when the reformer is started, the combustion amount is controlled based on a temperature measurement value at a predetermined position of the reformer.
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JP2010277844A (en) * | 2009-05-28 | 2010-12-09 | Toto Ltd | Solid oxide fuel cell |
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JPH05115770A (en) * | 1991-10-31 | 1993-05-14 | Tokyo Gas Co Ltd | Method for starting fuel reforming device |
JPH0765853A (en) * | 1993-08-20 | 1995-03-10 | Yamaha Motor Co Ltd | Methanol burner for fuel cell raw material reforming device |
JP2002356307A (en) * | 2001-03-26 | 2002-12-13 | Osaka Gas Co Ltd | Operation method for apparatus of producing hydrogen- containing gas |
JP2003151596A (en) * | 2001-11-16 | 2003-05-23 | Ebara Ballard Corp | Fuel cell generator system |
JP2004196610A (en) * | 2002-12-19 | 2004-07-15 | Rinnai Corp | System using reformer |
JP2006199543A (en) * | 2005-01-21 | 2006-08-03 | Mitsubishi Heavy Ind Ltd | Operation method of chemical conversion apparatus, operation method of fuel reforming apparatus and operation method of fuel cell |
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JPH05115770A (en) * | 1991-10-31 | 1993-05-14 | Tokyo Gas Co Ltd | Method for starting fuel reforming device |
JPH0765853A (en) * | 1993-08-20 | 1995-03-10 | Yamaha Motor Co Ltd | Methanol burner for fuel cell raw material reforming device |
JP2002356307A (en) * | 2001-03-26 | 2002-12-13 | Osaka Gas Co Ltd | Operation method for apparatus of producing hydrogen- containing gas |
JP2003151596A (en) * | 2001-11-16 | 2003-05-23 | Ebara Ballard Corp | Fuel cell generator system |
JP2004196610A (en) * | 2002-12-19 | 2004-07-15 | Rinnai Corp | System using reformer |
JP2006199543A (en) * | 2005-01-21 | 2006-08-03 | Mitsubishi Heavy Ind Ltd | Operation method of chemical conversion apparatus, operation method of fuel reforming apparatus and operation method of fuel cell |
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JP2010277844A (en) * | 2009-05-28 | 2010-12-09 | Toto Ltd | Solid oxide fuel cell |
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